Gray accepted a position as the defensive coordinator for the Tennessee Titans, the team announced on Saturday.
"I also want to thank Coach Brown and University of Texas," Gray said in a release. "I know the timing of this isn’t ideal, but this was something that I couldn’t turn down."
Gray's vacancy means Brown will launch a search for his seventh coaching hire of the offseason. Gray came to Texas on January 17 after coaching defensive backs for the Seattle Seahawks in 2010.
"We're obviously disappointed that Jerry's leaving, but at the same time, we're really excited about the wonderful opportunity he had to be the defensive coordinator of the Titans," Brown said in a release. "It is a chance for him to reunite with a lot of friends he went to the Super Bowl with who came up just one yard short of winning. That's the only place he would have left here for, and we want to wish him the best of luck."