The former Busted singer will appear in upcoming drama In God We Trust, according to The Sun.
He will be joined by his Fightstar bandmates Alex Westaway and Dan Haigh in the project.
Simpson is said to be playing a covert operations interrogator who later gets shot in the film.
It is currently unknown as to whether the role will be a main character or just a cameo.
Charlie Simpson recently told Digital Spy that online music culture is "disposable".
> Charlie Simpson interview: 'I'm hoping for US record deal'
Watch the trailer for In God We Trust below (contains graphic scenes):