This study presents the ankle ligament strains and ankle joint moments during an accidental injury event diagnosed as a grade I anterior talofibular ligament (ATaFL) sprain. A male athlete accidentally sprained his ankle while performing a cutting motion in a laboratory setting. The kinematic data were input to a three-dimensional rigid-body foot model for simulation analyses. Maximum strains in 20 ligaments were evaluated in simulations that investigated various combinations of the reported ankle joint motions. Temporal strains in the ATaFL and the calcaneofibular ligament (CaFL) were then compared and the three-dimensional ankle joint moments were evaluated from the model. The ATaFL and CaFL were highly strained when the inversion motion was simulated (10% for ATaFL and 12% for CaFL). These ligament strains were increased significantly when either or both plantarflexion and internal rotation motions were added in a temporal fashion (up to 20% for ATaFL and 16% for CaFL). Interestingly, at the time strain peaked in the ATaFL, the plantarflexion angle was not large but apparently important. This computational simulation study suggested that an inversion moment of approximately 23 N m plus an internal rotation moment of approximately 11 N m and a small plantarflexion moment may have generated a strain of 15–20% in the ATaFL to produce a grade I ligament injury in the athlete's ankle. This injury simulation study exhibited the potentially important roles of plantarflexion and internal rotation, when combined with a large inversion motion, to produce a grade I ATaFL injury in the ankle of this athlete.