Atwell made the transition to film roles early on, with her first major role coming in Woody Allen's 2007 film Cassandra's Dream, playing stage actress Angela Stark. Atwell's first major on-screen television role came in 2006 with BBC Two's miniseries, The Line of Beauty. In 2010 Atwell appeared in Channel 4's adaptation of William Boyd's, Any Human Heart, and later that year, Ken Follett's miniseries, Pillars of the Earth, which co-starred Eddie Redmayne; for which she was nominated for her first Golden Globe. Boyd, William (5 November 2010). «William Boyd on filming Any Human Heart». Kellaway, Kate (10 October 2010). «Hayley Atwell: 'The real me is a loner, a nerd and a bit overweight'». Minor, Jordan (9 October 2015). «Lego Marvel's Avengers bricks the Marvel Cinematic Universe». In a 2015 interview, Atwell discussed how her role as Peggy Carter influenced a then-recent tweet she made to her 319,000 Twitter followers about having her image digitally altered on the cover of a German magazine. Atwell played Agent Peggy Carter in the 2011 American superhero film Captain America: The First Avenger.

She also reprised the role of Peggy Carter in Avengers: Endgame. 2015 films Avengers: Age of Ultron and Ant-Man. Gomez, Patrick (7 January 2015). «5 things to know about Hayley Atwell». Rafanelli, Stephanie (2 July 2015). «Hayley Atwell: 'I've always felt quite genderless. Which is odd, because I have big boobs'». Shirey, Eric (29 July 2011). «Captain America: Super Soldier Video Game Review». Fox, Chloe (17 July 2011). «Action girl: Hayley Atwell interview». In September 2019 it was announced that Atwell will star in Mission: Impossible 7 and Mission: Impossible 8, both directed by Christopher McQuarrie and scheduled to be theatrically released in the United States on 23 July 2021 and on 5 August 2022, respectively. Robbins, Jason (13 September 2019). «Hayley Atwell Confirmed for Both Mission: Impossible 7 & 8». Screen Rant. In 2008, she appeared in the film The Duchess, which earned her a Best Supporting Actress nomination at the British Independent Film Awards.

In 2013, Atwell collaborated with Alexi Kaye Campbell and Jamie Lloyd again in a revival of The Pride at Trafalgar Studios; her performance gained her a second Olivier Award nomination for Best Actress. Atwell was also nominated for a WhatsOnStage Award for her role in The Pride. 2011 work her revival of The Pride. White, Leslie (21 August 2011). «Sizzling for England». White, Peter (12 July 2018). «Hayley Atwell & Tamara Lawrance To Star In David Heyman's BBC Drama The Long Song». Pisarra, Drew (24 July 2008). «Four More Residents of The Village». Dowell, Ben (13 July 2018). «Hayley Atwell, Lenny Henry and Tamara Lawrance cast in new BBC period drama The Long Song». Lane, Anthony (2 April 2018). «Hayley Atwell on the Superwomen of „Howards End“». Couto, Anthony (8 December 2016). «NYCC LIVE! Marvel Animation Panel ft. Ultimate Spider-Man, GOTG & More». Jusino, Teresa (13 May 2016). «Agent Carter Cancelled After Two Seasons, Mockingbird Not Flying in Marvel's Most Wanted». The series aired 13 episodes between October 2016 and January 2017; in May 2017, ABC announced it had been cancelled.

In February 2016, Atwell was cast in the ABC series Conviction. Later in the year, Atwell appeared as '415' in AMC Television's November 2009 miniseries, The Prisoner, a remake of the 1967-68 series by the same name. Atwell starred as Margaret Schlegel in BBC One's 2017-2018 miniseries, Howards End, based on the classic E.M. In 2019, Atwell starred opposite Tamara Lawrance in a three-part BBC adaptation of Andrea Levy's novel The Long Song, about a slave on a sugar plantation in 19th-century Jamaica. In 2013, Atwell starred in BBC Two's adaptation of William Boyd's espionage novel, Restless, before starring in «Be Right Back», an episode in Charlie Brooker's critically acclaimed science fiction television series, Black Mirror. The original rabbits were made with PVC rubber (and back then it wasn't phthalate-Free nude Video chat), and while today most rabbits are free nude video chat of pthalates — this material still is porous and allows places for microscopic bacteria to cling and aren't the easiest to sterilize.

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