The brothers learn from Bela which demon holds Dean's contract: a powerful demon named Lilith. Lilith is the very first demon ever made, with her soul being twisted by Lucifer himself in a spite against God for kicking him out. Lilith takes Bela's soul after her contract expires, but not before she warns Sam and Dean. The brothers, along with Ruby, track Lilith down and attempt to kill her. Lilith is unable to stop Sam on account of his mysterious abilities; however, Dean's contract expires and his soul is taken to Hell.
Dean is rescued from Hell and brought back by an angel of the Lord named Castiel. The rest of the season follows the brothers as they work with Castiel to stop Lilith's plan of breaking the 66 seals , which would allow the fallen archangel Lucifer, AKA "the Devil" or "Satan himself", to walk the Earth free once again. Sam and Dean's relationship is strained and Sam starts siding with Ruby over Dean.
He begins to give into his demonic side by drinking demon blood to become strong enough to defeat Lilith. He and Dean have a falling-out. Sam sides with Ruby in his obsessive quest to kill Lilith.
Dean makes a deal with the angels to save Sam, and learns that the angels want the Apocalypse to occur in order to rebuild Paradise on Earth. With aid from Castiel, Dean escapes and tries to stop Sam after learning that Lilith is, in fact, the last seal, but Sam kills her anyway, breaking open Lucifer's prison.
Ruby reveals her true colors as a demon loyal to Lucifer and Dean kills her. As the season ends, Lucifer's cage opens and he escapes from Hell. The fifth season revolves around the fight to stop Lucifer and save the world from the Apocalypse, inspired by events in the Book of Revelation. Throughout the season, while Castiel searches for God, Sam and Dean battle both angels and demons as they fight their destiny to become the vessels of Lucifer and Michael, respectively. They attempt to stop Lucifer by retrieving the Colt from the demon Crowley and attempting to kill Lucifer with it.
This fails as Lucifer can't be killed by the Colt, and they lose fellow hunters and friends Jo and Ellen in the process. Unable to defeat Lucifer, Sam and Dean, with information from the Trickster, revealed to be the archangel Gabriel, and with help from the demon Crowley, decided to collect the rings of the Four Horsemen of the Apocalypse , including Death, which act as the key to Lucifer's prison. In the end, Sam allows Lucifer to possess him and he kills Bobby and Castiel, who is now human. Sam then manages to regain control, thanks to his bond with Dean, and throws himself while possessed by Lucifer and Adam possessed by Michael into the Cage to trap Lucifer once more.
Castiel is resurrected by God and, more powerful than ever, resurrects Bobby and then returns to Heaven to restore order. Dean returns to his old girlfriend Lisa to live a normal life. Sam is next shown mysteriously free of the Cage, watching his brother eating dinner in the house with Lisa and her son Ben. Beginning with this season, Kripke did not return as showrunner, but still remained as a hands-on executive producer, leaving executive producer Sera Gamble to take over the reins.
The sixth season begins a year after the conclusion of the fifth season, with Dean living a somewhat happy life with Lisa and Ben. When an emotionless Sam returns to Dean, he is forced to leave his new life behind and work with his resurrected grandfather Samuel to capture Alpha monsters for Crowley.
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The brothers are unable to get much help from Castiel since his time is occupied by a civil war raging in heaven against the archangel Raphael. Dean does not trust Samuel and his suspicions are confirmed when he finds Samuel working with demons to discover the location of Purgatory. Dean discovers that Sam's soul is still in the Cage, so he implores the Horseman Death to retrieve it. To ensure Sam does not remember his time in the Cage, Death blocks that part of Sam's memory using a mental wall. The season's second half revolves around the so-called Mother of All, which ultimately leads to events which prove that Castiel is behind the circumstances of Sam's return, the hunt for the Alpha monsters, and the search for Purgatory and was working with Crowley the entire time.
When the brothers try to stop Castiel, he brings Sam's memory of the Cage back and proceeds with his plan, absorbing all the souls from Purgatory and pronouncing himself God, having ascended beyond a mere angel. After absorbing souls from Purgatory and declaring himself God, Castiel begins to punish all the wrongdoers in the world. He discovers that he absorbed the Leviathans , who are attempting to break free of his vessel. Sam and Dean manage to return most of the souls to Purgatory but fail to return the Leviathans, who seemingly kill Castiel before vanishing and inhabiting the bodies of many different people around the world.
Sam and Dean learn that their weakness is Sodium Borate also known as Borax , though it has minimum effectiveness on the Leviathan leader Dick Roman. After Roman kills Bobby, Dean becomes obsessed with taking the Leviathans down and learns of a facility they are building, only to discover that it is a facility to cure cancer. The spirit of Bobby later confirms that while they are curing disease, they are doing it as part of their plan to turn humanity into the perfect food source.
With Castiel and Kevin's help, the brothers learn that the only way to kill the Leviathans is with the "bone of a righteous mortal washed in the three bloods of the fallen" and set out to find the three bloods. Kevin can read the word of God and helps Sam and Dean decipher it to stop the Leviathans. Eventually, Dean and Castiel kill Dick but are dragged into Purgatory as a result, while Sam is left alone to deal with Crowley, who plans to rise to power now that the Leviathans are disorganized. Key plot points presented in the season were Sam struggling with the constant hallucinations of Lucifer and the ghost of Bobby "haunting" Sam and Dean through his alcohol flask.
Bobby's rage toward Dick Roman slowly causes him to become a vengeful spirit , and Sam and Dean ultimately deal with this by burning the flask at his request, thus destroying Bobby. One year after being dragged to Purgatory, Dean returns to Earth without Castiel, carrying inside his body the soul of a vampire named Benny. The two brothers begin a fight against Crowley to find the Demon Tablet and lock the Gates of Hell, thereby trapping all demons in Hell.
The brothers use Kevin Tran to help them read the tablet and accomplish this.
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Castiel is brought back by an angel named Naomi, and takes possession of the Angel Tablet to break her control of him when she tries to use him to kill Dean. While Kevin works on the tablet, Sam and Dean have an unexpected encounter with their paternal grandfather, Henry Winchester, who was a member of the Men of Letters, an organization dedicated to gathering supernatural knowledge; his disappearance in was actually him using a time-travel spell to go to the future and escape an attack by the demon Abaddon.
Henry is killed protecting his grandsons, but he provides them with access to the Men of Letters bunker, a storehouse for several supernatural artifacts and books, which the Winchesters subsequently adopt as a new 'home'. Kevin translates three trials that must be completed in order to lock the Gates of Hell for good, but although Sam completed the first two, Dean ends the trials before the third can be finished as completing the trials would kill Sam. Unfortunately, Castiel is tricked by the angel Metatron into completing another series of trials that would have allegedly locked all angels in Heaven, but actually banished every angel apart from Metatron to Earth, the season ending with millions of angels falling from the sky and Castiel stripped of his Grace.
In the first half of the ninth season, the angels have fallen to Earth and two angel factions are warring against each other while hunting Castiel. Rogue angels roam the Earth causing trouble. Castiel is now human and has to adjust to his new life while Crowley is held prisoner by Sam and Dean who are trying to use an old blood ritual to turn demon Crowley back into a human. Sam is left near-death from the Trials of God and Dean is forced to let an angel, claiming to be Ezekiel, possess Sam to heal him from the inside. Dean must hide Ezekiel's presence from Sam so that he won't expel him and die while also keeping Castiel away at Ezekiel's demand.
The brothers search for a way to return the angels to Heaven. Eventually it is revealed that Ezekiel is actually Gadreel , the angel who let Lucifer into the Garden of Eden. Gadreel murders Kevin Tran and escapes to join Metatron, while Castiel regains his powers after taking the Grace from another renegade angel. With Crowley's help, Sam expels Gadreel, but the experience causes Sam and Dean to split up while letting Crowley go as part of the deal Dean made for him to save Sam.
In the second half, Dean begins searching for both Gadreel for revenge and the First Blade to kill Abaddon with the help of Crowley. Despite being warned of terrible repercussions, Dean takes on the Mark of Cain in order to be able to wield the First Blade.
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After healing Sam completely, Castiel begins a search of his own for Metatron, believing him to be the key to reversing the expulsion of the angels. Metatron begins trying to unite all the angels under his rule while Castiel leads other angels against him to retake Heaven. Eventually Dean kills Abaddon and Castiel defeats Metatron after a repentant Gadreel sacrifices himself to let Castiel confront Metatron directly, but Metatron kills Dean, causing Dean to become a demon due to the influence of the Mark of Cain. In the tenth season, after being resurrected by the Mark of Cain, Dean is now a demon, working alongside Crowley.
Meanwhile, Sam continues to search for Dean. After Dean refuses to follow Crowley's order and embarrasses him in front of his demon followers, Crowley gives Sam his brother's location. Later, Sam, with the help of Castiel, cures Dean by using sanctified human blood. After being cured, Dean is reminded by Castiel that the Mark of Cain is still a problem. Dean and Sam help Castiel track down his vessel's Jimmy's daughter, Claire.
Dean ends up slaughtering several men who are keeping her captive and loses control of the Mark, a nightmare he previously had. Meanwhile, a mysterious new witch comes into play, being revealed to be Crowley's mother, Rowena. A large focus of the season is Dean's quest to overcome the Mark of Cain and have it removed if possible.
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Sam needs help in reading and using the tome, and turns to Rowena for help. He requests help from Charlie, too, who decodes the text but is murdered by the Steins, a family that has secretly controlled much of history. After massacring the Steins, nearly killing Castiel and getting another hunter killed, Dean starts despairing of being free of the Mark, causing him to turn to Death for help. Death proposes putting Dean in isolation away the Earth, but insists Dean must kill Sam, who otherwise would work to bring Dean back.
Sam and Dean both agree that it is for the good of the world. At the last moment however, Dean seemingly kills Death instead to save Sam.
Oblivious to the dangers, Rowena successfully casts the spell to remove the Mark and unleashes the Darkness, a primordial evil that had been kept away by the Mark. Rowena also places Castiel under a spell so he attacks Crowley as she escapes with the Book of the Damned. While Crowley's taking care of Amara, feeding her with souls, the brothers are, alongside Castiel, trying to find a way to kill The Darkness.
In order to find out more about Amara, Castiel asks Metatron for help, and he says that in order to create the world, God had to sacrifice his sister, The Darkness. To face the most dangerous creature they've crossed paths with so far, the brothers ask for Lucifer's help. Lucifer claims he's the only one that can beat Amara, but in order to do so, he needs to possess Sam's body.
Later, it's revealed that Castiel said "yes" at the last second, and that Lucifer is now possessing his body. When nothing works to get rid of The Darkness, Amara claims that God must appear himself to see her destroying everything He created and loves. Meanwhile, Chuck returns and reveals himself to Metatron, telling him he is God.
Then, he reveals himself to the Winchesters and they all decide to seal Amara. Rowena, who had cast a spell that made her immortal, helps them with a spell, while Crowley and Lucifer use the demons and angels in a combined attack against Amara. When Chuck tried to seal Amara, she resisted, stopping the Winchesters, apparently killing Lucifer and gravely wounding Chuck. Amara warns that Chuck is not dead yet because he is going to watch her destroy everything ever created.
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