Continued acclaim ensued with the independent films Nowhere Boy (2009), in which he portrayed Paul McCartney, Bright Star (2009), and Death of a Superhero (2011).

He subsequently appeared in a few more television films, including the lead roles in Bobbie's Girl, The Miracle of the Cards (based on the story of Craig Shergold) and Stig of the Dump.

In 2008, Brodie-Sangster had a role in director Jane Campion's film Bright Star, a love story about John Keats and his lover Fanny Brawne.

He also starred as Paul McCartney in Nowhere Boy, a film directed by artist Sam Taylor-Wood, about the teenage years of John Lennon.

[10] In 2015, he began providing the voice of John Tracy in ITV's remake of Gerry Anderson's puppet series Thunderbirds Are Go (2015–2020).

[11] In BBC2's 6-part television adaptation of Wolf Hall (on BBC2 from 21 January 2015), Brodie-Sangster portrayed Rafe Sadler, the ward of Thomas Cromwell.

[13] In 2017, Brodie-Sangster began portraying Whitey Winn in the 2017 Netflix western drama miniseries Godless, created by Scott Frank.

Brodie-Sangster began the 2020s with a role as chess player Benny Watts in the Netflix miniseries The Queen's Gambit (2020), marking his second collaboration with Frank.

[14] His performance as Watts earned Brodie-Sangster a nomination for the Primetime Emmy Award for Outstanding Supporting Actor in a Limited Series or Movie.