[2] Alexandrou's acting career began in 1996, when he auditioned successfully for the role of Martin Fowler in the BBC One soap opera EastEnders.
The character was created shortly after the show's inception in 1985, with the role becoming vacant following the departure of actor Jon Peyton Price in 1996.
He and Natalie Cassidy, who played his on-screen wife Sonia Fowler, left on 2 February 2007 (to tie in with the exits of Wendy Richard and Ray Brooks).
[11] In October 2008, Alexandrou appeared in All Quiet on the Western Front at the Nottingham Playhouse, prior to a UK tour of the production.
[12] In October 2009, Alexandrou joined up with EastEnders cast members, Natalie Cassidy (Sonia Jackson) and Nina Wadia (Zainab Masood), to star in comedy shorts for BBC Raw Words.
[14] He appeared in the role of The Man in John Goodrum's play The Black Veil a thriller adapted from a Charles Dickens short story.
[13] In 2011 Alexandrou took part in the BBC Learning project, Off By Heart Shakespeare, where he played Mercutio from Romeo and Juliet delivering the speech; "'tis not so deep as a well".
Rehearsals were recorded by BBC World Service and James Alexandrou's performance as Iago featured in their programme The Why Factor.