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."
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.
Armie Hammer as Christian Grey
Copper hair, strong build, steely gray eyes ... Armie Hammer would make the perfect Christian Grey. He's 25, just the right age to pull off 27-year-old Grey's air of success and boyish charm, and he can go from serious and sexy smirk in a second.<br /> <i> Backups: Ryan Gosling, Michael Fassbender, Chris Pine, Henry Cavill</i>
Elizabeth Olsen as Anastasia Steele
Olsen breakout role in "Martha Marcy May Marlene" proved she can play frightened and confused like a pro. But it's her piercing blue eyes that seal the deal -- darken her hair a few shades, and she is not-so-innocent recent college grad Ana.<br /> <i>Backups: Dakota Fanning, Saoirse Ronan, Alexis Bledel, Emma Stone</i>
Evan Rachel Wood as Kate Kavanagh
Ana's inquisitive roommate Kate has strawberry blonde hair and a fierce attitude. Wood often plays older than her 24 years, but would make a believable mature recent college grad with sex appeal. <br /><i>Backups: Carey Mulligan, Mia Wasikowska, Blake Lively, Ari Graynor</i>
Michael Trevino as Jose Rodriguez
Young photographer and college student Jose adores Ana and desperately wants to be more than just friends, but the arrival of Christian Grey solidifies his place as a pal. "The Vampire Diaries'" Trevino has proven he can play tortured, and his good looks make him a nice threat for Mr. Grey. <br /><i> Backups: Taylor Lautner, Penn Badgley, Mark Salling</i>
Michael Keaton as Ray Steele
Ana's stepdad Ray is ex-military and likes the simpler things in life, like baseball and fishing, but he's got a soft spot for his little girl. Ray's role isn't huge, but Keaton could easily pull off playing the reserved, protective pop. <br /><i> Backups: Ed Harris, Bryan Cranston, Jeffrey Dean Morgan</i>
Mary Steenburgen as Carla
Ana's mom Carla is a hopeless romantic, but also fairly unlucky in love. Ray was her second husband who Ana stayed to live with when she ran off with #3. Now on #4, she's hoping her daughter won't make the same mistakes. <br /><i>Backups: Patricia Clarkson, Marcia Gay Harden, Teri Hatcher</i>
Jimmy Smits as Jose Rodriguez Sr.
Jose's dad and Ana's dad Ray were old army buddies, reunited when their kids became friends at college. Jose Sr. also desperately wants Ana and his son to get together, and Smits can play convincing in his sleep. <br /><i> Backups: Danny Trejo, Edward James Olmos</i>
Susan Sullivan as Grace Trevelyan-Grey
Christian's mother Grace -- a pediatrician who adopted him at the age of 4 -- is smart, sweet and very high society. Sullivan's poise would be perfect, but it's her ability to play sadness and fierce maternal instincts that would come in handy. <br /><i>Backups: Susan Sarandon, Joan Allen</i>
Stellan Skarsgard as Carrick Grey
Carrick is a successful lawyer and businessman who makes his family's best interests a top priority. He's soft spoken, but still has presence -- Skarsgard's soulful eyes would definitely come in handy for the more emotional moments. <br /><i>Backups: Harrison Ford, Victor Garber</i>
James Franco as Elliot Grey
Christian's older adopted brother, Elliot, is a good time guy and a real ladies man -- Franco could pull off both -- who's always giving his little brother a hard time for his single status ... until Christian meets Ana. <br /><i> Backups: James Marsden, Zach Gilford</i>
Lucy Hale as Mia Grey
Christian's little sister Mia has always been the only woman who can give him a hard time and get away with it. Lucy Hale could play the energetic brunette in a second. <br /><i>Backups: Leighton Meester, Emmy Rossum, Nina Dobrev</i>
Christopher Meloni as Taylor
Christian Grey's most trusted security man, Taylor is ex-FBI and the strong, silent type ... but he reserves a smile here and there for Ana. <br /><i>Backups: David Morse, Bruce Willis</i>
Helen Mirren as Mrs. Jones
Christian's housekeeper Mrs. Jones is also a mother figure of sorts, keeping his swanky penthouse home tidy, cooking all meals and keeping the refrigerator stocked with his favorites. <br /><i>Backups: Cybill Shepherd, Jane Seymour, Julie Andrews
Sharon Stone as Elena
Christian's Mrs. Robinson -- the woman who welcomed him into the kinky world of BDSM at a very young age -- needs to be a predator, but still sexy in her older age. Sharon Stone fits the bill. <br /><i>Backups: Ellen Barkin, Meg Ryan, Morgan Fairchild
Colin Firth as Dr. Flynn
Dr. Flynn is the voice of reason in Christian's life, and they have more than just a therapist-patient relationship. Flynn is a confidant and charming in his own right. <br /><i>Backups: Clive Owen, Ralph Fiennes, Guy Pearce, Robert Downey Jr.</i>