Talus morphology (shape and size) plays a pivotal role in talocrural joint function. Despite its importance, the relationship between talus morphology, particularly the talar dome, and dynamic, in vivo talocrural function is poorly understood. Understanding these form–function relationships in a healthy cohort is essential for advancing patient-specific treatments aimed at restoring function. Nine participants (five females) hopped on one leg while biplanar videoradiography and ground reaction forces were simultaneously collected. Three-dimensional bone models were created from computed tomography scans. Helical axes of motion were calculated for the talus relative to the tibia (rotation axes), and a cylinder was fitted through the talar dome (morphological axis). Bland–Altman plots and spatial angles were used to examine the level of agreement between the rotation and morphological axes. A shape model of 36 (15 females) participants was established, and a cylinder fit was morphed through the range of ±3 standard deviations. The rotation and morphological axes largely agree regarding their orientation and location during hopping. The morphological axes were consistently oriented more anteriorly during landing than the rotation axes. Some shape components affect talar dome orientation and curvature independent of size. This suggests that besides bone size, the shape of the talar dome might influence the movement pattern during locomotion. Our findings may further inform talocrural joint arthroplasty design.