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Williams was born and raised in New Canaan, Connecticut, and is the daughter of former NBC Nightly News anchor and managing editor Brian Williams and Jane Gillan Stoddard, a TV producer. She graduated from Yale University in 2010.[3] While at Yale, Williams was a member of the improv comedy troupe Just Add Water for four years, as well as being a part of the YouTube series College Musical, and was inducted by St. Elmo.

In 2010, Williams performed a mashup of “Nature Boy” set to RJD2’s “A Beautiful Mine”, the theme song for the television series Mad Men. The YouTube video of the performance received widespread praise on the Internet, and convinced Judd Apatow that she should be given a part in the HBO series Girls. She was cast shortly after and credited her experience at Just Add Water for passing the audition. Girls premiered on April 15, 2012.

Williams wrote a series of Funny or Die sketches, in which she starred as newlywed Kate Middleton, with English actor and model Oliver Jackson-Cohen as Prince William, Duke of Cambridge. Williams appeared as Danielle in an episode of the third season of The League titled “The Guest Bong”.

Williams has appeared as a recurring character, Cheryl, in the CollegeHumor series Jake and Amir.On December 4, 2014 she starred in the title role on NBC’s live television presentation of the musical Peter Pan Live!

Williams began dating Ricky Van Veen, the co-founder of CollegeHumor in 2011. They became engaged in 2014.On September 19, 2015, Williams and Van Veen wed in a private ceremony at Brush Creek Ranch in Saratoga, Wyoming. Tom Hanks officiated the ceremony.