In November 2011, DeVitto was confirmed to have a recurring role in the CW fantasy drama series "The Vampire Diaries" as Dr. Meredith Fell, who is fascinated by Alaric Saltzman (Matthew Davis), when she notices how quickly he recovers from an injury. She portrayed Margo in the comedy-drama film "Cheesecake Casserole" (2012), released on July 3, 2012. In November 2012, it was reported that she had signed on to star as Maggie Hall in the seventh season of the Lifetime drama series "Army Wives". Maggie Hall is a mother of two and former soldier who moves to Fort Marshall with her family. On September 24, 2013, Lifetime announced the show's cancellation, it honored the show with a two-hour retrospective special with the cast members which aired in 2014. She had a lead role as Jennie Stanton in the Hallmark Channel television film "Best Christmas Party Ever" in 2014.In August 2015, DeVitto signed on to star in the NBC medical drama series "Chicago Med". She was cast as Dr. Natalie Manning, the ED pediatrician. She has also appeared as Dr. Natalie Manning in "Chicago P.D." and "Chicago Fire". She portrayed Angie in the psychological thriller "The Hoaxing" (2018), a short film that she also helped produce. In 2019, she produced a documentary film, "Saving Daisy" that follows Daisy Coleman’s journey of healing from lifelong trauma and PTSD. She starred in Hallmark Channel's television film "Write Before Christmas" (2019) alongside Chad Michael Murray. The film centers around Jessica, portrayed by DeVitto, who sends Christmas cards to five people who have impacted her life. "The New York Times" placed the film on its list of "Five Holiday Movies Worth Bingeing This Season". She played Cathy in the thriller film "Divertimento" (2020) alongside Kellan Lutz and Ola Rapace.