Upon graduating in 2000, Yusef was offered a role in Fred Schepisi's award-winning film Last Orders, playing the younger self of Bob Hoskins' "Ray" and working with British actors Sir Michael Caine, Dame Helen Mirren, Ray Winstone, David Hemmings, and Tom Courtenay.

In 2006, Yusef's performance as Mercutio in Bill Bryden's Romeo and Juliet at the Birmingham Rep was heralded as "sparkl[ing]" and "promisingly imaginative".

In 2008, Yusef appeared in the title role of a New York off-off Broadway production of Richard III, and was described by Backstage as "a superlative actor" and "magnetic". Anatol has since remained in New York City. He has worked both throughout New York City, and at The Studio Theatre in Washington, D.C., his most recent production being A Movement of the Soul, playing Thomas Hopkins Gallaudet, for which he learned American Sign Language.

In 2010 he was cast as Meyer Lansky in HBO's Boardwalk Empire, first appearing in Episode 7 of Season 1, "Home" and recurring throughout the remainder of the series. In an interview with The Morton Report, Yusef described Lansky as self-educated, a massively intelligent overachiever and "a ruthless, ruthless man". Anatol's characterization of Mr. Lansky has been recognized in many publications, including author and critic Clive James's article on Martin Scorsese, as well as Michael Noble's review of the show on Den of Geek.

In 2014 he appeared in Channel 4's BAFTA-nominated Southcliffe, receiving special mention in an article by IndieWire on the best TV episodes of 2014.