Cloud, Repeaters (both 2010), Charlie Zone (2011), Ferocious (2013), Chokeslam (2016), Tone-Deaf (2019), and Some Other Woman (2023), as well as supporting roles in The Haunting in Connecticut (2009), The Age of Adaline (2015), Freaks (2018) and There's Something Wrong with the Children (2023).

In 2005, at age 19, Crew landed her first onscreen acting role as Polly Brewer on the ABC teen drama Life as We Know It.

She made a cameo appearance as a sorority sister in an episode of Smallville, a television series based on the DC Comics character Superman.

Despite negative reviews from critics, the film opened in second place at the North American box office, ultimately grossing $77.5 million worldwide.

Later that year, she starred in the sci-fi crime thriller Repeaters as Sonia Logan, a drug addict in rehab who becomes trapped in a time loop.

Crew guest-starred on the USA Network legal drama Suits, as an expert hacker who has stolen money from her father's company.

From 2014 to 2019, Crew starred as venture capitalist Monica Hall on the HBO comedy Silicon Valley, created by Mike Judge.

During the first season, her character was originally an assistant to Peter Gregory (played by Christopher Evan Welch), but in the second season she becomes an associate partner with Laurie Bream (played by Suzanne Cryer) after Welch's death in 2013, and later leaves Bream Hall to join Pied Piper as its CFO and business advisor.

She guest-starred on the second season of the CTV police procedural drama Motive as Robin Keaton, a young widowed mother who becomes engaged unknowingly to the man responsible for the murder of her son's father.

In her third collaboration with director Carl Bessai, she starred as seductive librarian Izzy Fontaine in the crime comedy Bad City, which premiered at the Oldenburg International Film Festival on September 10, 2014.

The film was nominated for nine Leo Awards, including Best Feature Length Drama and Best Supporting Performance by a Female in a Motion Picture for Crew.

Crew co-starred with musical duo Aly & AJ in the comedy drama Weepah Way for Now, which premiered at the Los Angeles Film Festival on June 16, 2015.

She co-starred with Michael Shannon in the western drama Poor Boy, playing a roller girl who moonlights as a prostitute.

She later co-starred with Ed Harris and Amy Madigan in the black comedy thriller A Crooked Somebody, playing a woman whose father was murdered when she was a child.

She co-starred with Adam Brody in the horror Isabelle, playing a woman who begins seeing a supernatural entity following the death of her stillborn son.

She co-starred opposite Tom Felton and Ashley Greene in the psychological thriller Some Other Woman, which premiered at the Mammoth Film Festival on March 3, 2023, to mixed reviews from critics.