The 60-year-old actor will portray defense attorney Robert Shapiro on the FX miniseries. Travolta will also act as producer, with American Horror Story co-creators Ryan Murphy and Brad Falchuk as executive producers.
American Crime Story: The People vs. O.J. Simpson will examine the trial of former NFL star O.J. Simpson. The football player was accused of murdering wife Nicole Brown Simpson in 1994, but was acquitted of the crime in 1995.
Cuba Gooding Jr. will star as Simpson, with Sarah Paulson as head prosecutor Marcia Clark. David Schwimmer will portray defense attorney Robert Kardashian, who collaborated with Shapiro on the accused's team of lawyers.
American Crime Story is being envisioned as an anthology series, and a companion show to American Horror Story. Season one will consist of 10 episodes written by creators Scott Alexander and Larry Karaszewski, and premiere in 2015.
Travolta's last television role was Vincent "Vinnie" Barbarino on 1970s sitcom Welcome Back, Kotter. The actor subsequently appeared in a number of films, including Pulp Fiction and Hairspray, and is scheduled for In a Valley of Violence in December.