The 33-year-old actress - who gave birth to twins, the fifth and sixth children she raises with partner Brad Pitt, earlier this month - is said to be in final negotiations with studio bosses to play the feline villain who first appeared in the Batman comics.
Angelina has already been approved for the role by Julie Newmar, who played Catwoman in the "Batman" TV series from 1966 to 1968.
Julie, now 74, said: "Angelina would own the part. My industry friends tell me she has already made inquiries about the role. I can understand how it would pique her interest. Catwoman is Batman's one true love."
"She is tremendously popular with women because she's both a heroine and a villainess."
Since the TV series, other actresses to take on the role of Catwoman include Michelle Pfeiffer in 1992 movie "Batman Returns," while Halle Berry's portrayal of the villain in 2004 film "Catwoman" was panned by critics worldwide.
Angelina was recently tipped to be starring in "The Thomas Crown Affair 2" alongside Pierce Brosnan, but has been ordered by bosses to put on 28 lbs for the role.