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According to People, the actress has moved out of the Brooklyn brownstone she purchased with late actor Heath Ledger and into a Brooklyn loft with her boyfriend.
Williams, 32, is renting the loft in a converted warehouse that overlooks the Manhattan skyline, and Segel recently moved in with the single mother.
"She is renting it, but he stays there," a source told People magazine.
The My Week with Marilyn star and the How I Met Your Mother actor, also 32, met through Busy Philipps -- Williams' best friend and Segel's former Freaks and Geeks costar -- and have been dating since the beginning of the year. They've been spotted together and with Williams' daughter Matilda many times and have not been especially shy about their romantic relationship.
A source tells People that Segel star is "totally smitten" with Williams. "It's like the first girl he's ever been this way with," the source confirmed.
Williams and Ledger bought their Brooklyn townhouse in 2005, when their daughter Matilda was a newborn. (She turns 7 on Sunday.) Purchased for $3.6 million, the brownstone is now believed to be worth up to $4.2 million.
After Ledger died in January 2008 from a drug overdose -- five months after he and Williams separated -- the actress kept the brownstone and has quietly raised their daughter there ever since.
Now it sounds like Williams and Segel are getting quite serious with each other. Could this be the first step toward marriage?