The Oscar-winning actress has been reading the "mummy porn" novel on set of her latest film Maleficent and now wants a part, according to The Mirror.
A source reportedly told them: "She knows the film is bound to be a huge hit."
Is Angelina Jolie your idea of Anastasia Steele?
The Twilight-inspired novel, written by British author James, follows a young college student as she embarks on a BDSM relationship with an older businessman.
Jolie being cast as the leading lady Anastasia Steele - who's described as pale, with long dark hair and blue eyes too big for her face - is highly unlikely, partly because she's 37-years-old (not 'young' college student age) and also because Steele is a virgin at the beginning of the story.
More likely names that have been thrown into the ring include younger actresses with more innocent reputations, such as Lilly Collins, Emma Watson, Alexis Bledel, Nina Dobrev, Kristen Stewart, Rachel McAdams, Emilia Clarke, Amanda Seyfried and Ashley Greene.
The International Business Times recently reported that Harry Potter actress Watson is "is one of the prime choices for the role".
Producers of The Social Network, Mike De Luca and Dana Brunetti, will bring the film to screen.
It was also recently rumoured Jolie would be directing the film. Deadline.com journalist Mike Fleming wrote while breaking the news of Jolie's potential involvement: "I've heard rumors about the possibility of Angelilna Jolie having a conversation or two about directing it." However, her reps said that no discussions occurred.
As for Ana's seducer Christian Grey, the fictional heart throb was recently imagined in the flesh with the help of image-generating software and descriptions from women who have read the book, while Chris Pine and True Blood's Alexander Skarsgård have been linked to the screen adaptation.