Chronic ankle instability (CAI) results in longstanding symptoms and subjective feelings of “giving way” following initial ankle sprain. Our purpose was to identify differences in joint coupling and variability between shank internal/external rotation and rearfoot inversion/eversion throughout the gait cycle of CAI subjects and healthy controls. Twenty-eight young adults participated (CAI, n = 15, control, n = 13). Kinematics were collected while walking and jogging on a treadmill. A vector coding method in which direction (θ) and magnitude of the angle-angle relationship and stride-to-stride variability (VCV) in shank-rearfoot coupling were calculated. In walking, the CAI group demonstrated lower θ, indicating a greater proportion of rearfoot-to-shank motion, compared with the control group in early and late swing. The CAI group had higher magnitude, indicating greater combined motion between the two segments, in early swing, but lower magnitude, indicating less combined motion, during late swing. The CAI group also had lower VCV measures, indicating less stride-to-stride variability during stance. In jogging, the CAI group had lower θ measures than the control group during stance and swing. Differences in shank-rearfoot coupling of the CAI group may be related to changes in sensorimotor control and lead to further instances of instability.