The actors, who played Bart McQueen and Joel Dexter respectively, finished filming with the Channel 4 show late last year.
Viewers of E4's first look screening saw Bart and Joel decide to leave the village forever in tonight's (January 8) episode as they went on the run, deserting their girlfriends Sinead O'Connor (Stephanie Davis) and Theresa McQueen (Jorgie Porter).
The pair had teamed up to steal cash from Brendan Brady (Emmett Scanlan), but when the bad boy caught them in the act, he ordered them both to disappear.
Bart was also potentially in hot water over his involvement in the sixth formers' devastating mini-bus crash, after Esther Bloom (Jazmine Franks) had given a new statement to the authorities.
Speaking exclusively to Digital Spy about bowing out as Bart, Clarke commented: "Hollyoaks has been a great stepping stone in my career, and leaving the show is one of the hardest decisions I've had to make so far.
"I believe I am at a great age to progress my career further. I am excited to see what the future brings. I hope to be involved in films and some period dramas.
"I would like to thank my family for their support and would also like to thank all my fans for all the great comments and good wishes they have sent me for my future career."
Clarke joined the cast of Hollyoaks in summer 2010, when his character joined the McQueen household and quickly struck up a close relationship with transgender teen Jasmine Costello. Bart's later storylines saw him begin dating Sinead and fall off the rails with a growing cannabis habit.
Still, meanwhile, signed up as Joel in late 2011 and his storylines have often seen 'Scottish Foxy' run into trouble while trying to impress Brendan.
Hollyoaks viewers watching at Channel 4 pace will see Bart and Joel's exit story play out tomorrow (January 9) at 6.30pm. Get the Inside Soap magazine on your iPhone or iPad