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The news was announced at Disney's fan expo D23 on Saturday.
Although Harington wasn't in attendance, Harington's Stark stepbrother in 'GoT', actor Richard Madden was a part of the cast announced at San Diego Comic-Con, along with Angelina Jolie.
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Harington, best known for his role of Jon Snow in 'GoT', will play a non-eternal character named Dane Whitman, aka the Black Knight, in the upcoming superhero film 'The Eternals'. Madden had previously been announced to play Ikaris in the movie.
'Dunkirk' fame Barry Keoghan was also added to the cast as an Eternal named Druid.
The casting news came a day after Deadline reported that Harington was headed to the Marvel Cinematic Universe where he will make his next film.
Marvel Studios President Kevin Feige also confirmed that Gemma Chan will play Sersi in the film.
The upcoming superhero film also stars previously announced cast members Angelina Jolie as Thena, Salma Hayek as Ajak, Kumail Nanjiani as Kingo, Lauren Ridloff as Makkari, Brian Tyree Henry as Phastos, and Lia McHugh as Sprite.
All the cast members, excluding Harington, appeared at 'The Eternals' presentation at D23.
The film centres on a race of never-aging, never-fading figures. The Eternals were created by the powerful godlike creatures known as the Celestials, and since their birth thousands of years ago, they've kept watch over the Earth throughout human history.
The superhero flick is being directed by Chloe Zhao, which is set for release on November 6, 2020.
Meanwhile, in May, Harington took a brief break from the spotlight, checking into a wellness retreat to deal with personal issues ahead of the 'GoT' finale. He is currently nominated for an Emmy for his work as Jon Snow in the show's final season.
Madden and Harington's 'Game of Thrones' sister Sophie Turner is also part of the MCU. She plays the role of Jean Grey in the X-Men films and reprised her role in 'Dark Phoenix' in June.