 Head coach Dirk Koetter named Grimes and Alterraun Verner the starting cornerbacks to begin the regular season, ahead of Vernon Hargreaves, Josh Robinson, Jude Adjei-Barimah, and Johnthan Banks.On December 24, 2016, Grimes recorded a season-high nine solo tackles in the Buccaneers' 31–24 loss at the Indianapolis Colts in Week 16.The following week, Grimes made a season-high four pass deflections, recorded four combined tackles, and returned an interception for a touchdown during a 17–16 victory against the Carolina Panthers in Week 17.