Accola had guest appearances in a number of television series such as How I Met Your Mother, Supernatural and Drop Dead Diva. In July 2009 Accola starred in the independent horror film Deadgirl which centers on two high school boys who discover an immortal woman in an abandoned asylum. That same year again Accola had a bit-role in The Hannah Montana Movie. In 2009 Accola was cast in The CW television series The Vampire Diaries as Caroline Forbes, a teenage vampire. The series was an immediate success with the series premiere reaching 4.91 million viewers. Critical reception was positive. In June 2012 Accola joined the dramedy YouTube series Dating Rules From My Future Self as Chloe Cunningham a 26-year-old girl who believes love does not exist. The series centers on a girl receiving romance advice from herself ten years in the future via text message. The first season of the series went on to receive over 14 million views.[clarification needed]
Accola began dating musician Joe King of The Fray after they met at a Super Bowl event in February 2011. They became engaged in May 2013, and married on October 18, 2014 in New Orleans, Louisiana. Upon her marriage, Accola became a stepmother to King's two daughters from his first marriage, Ava and Elise.