The couple - who got engaged last July after dating for one year - reportedly broke up last month although the `Inception` actor is said to be desperate to rekindle their relationship.
A source told the Metro newspaper: "Tom and Charlotte broke up last month. He has been calling her a lot to try to patch things up."
Tom, 33, and 28-year-old Charlotte first met on the set of the TV adaptation of `Wuthering Heights` when they were cast as star-crossed lovers before going on to work together again in television drama `The Take`.
Speculation about the couple`s relationship has been mounting after Tom failed to make an appearance at Sunday`s (13.02.11) BAFTAs where he won the Orange Wednesdays Rising Star Award.
He is said to have sent an apology blaming "personal commitments" for his absence.
The actor - who has signed to star as a villain in Christopher Nolan`s latest Batman film `The Dark Knight Rises` was previously married to Sarah Ward from 1999 to 2004.
He has a two-year-old son Louis Thomas Hardy with ex-girlfriend Rachael Speed.
Tom - who battled alcoholism and a crack cocaine addiction in his early-to mid-twenties - revealed last year he had relationships with men when he was younger.
He said: "I`m an actor for f**k`s sake. I`ve played with everything and everyone. I love the form and the physicality, but now that I`m in my thirties, it doesn`t do it for me. I`m done experimenting."