Understanding how motor units (MUs) contribute to skeletal mechanical force is crucial for unraveling the underlying mechanism of human movement. Alterations in MU firing, contractile and force-generating properties emerge in response to physical training, ageing or injury. However, how changes in MU firing and twitch properties dictate skeletal muscle force generation in healthy and impaired individuals remains an open question. In this work, we present a MU-specific approach to identify firing and twitch properties of MU samples and employ them to decode musculoskeletal function in vivo. First, MU firing events were decomposed offline from high-density electromyography (EMG) of six lower leg muscles involved in ankle plantar-dorsi flexion.We characterized their twitch responses based on the statistical distributions of their firing properties and employed them to compute MU-specific activation dynamics. Subsequently, we decoded ankle joint moments by linking our framework to a subject-specific musculoskeletal model. We validated our approach at different ankle positions and levels of activation and compared it with traditional EMG-driven models. Our proposed MU-specific formulation achieves higher generalization across conditions than the EMG-driven models, with significantly lower coefficients of variation in torque predictions. Furthermore, our approach shows distinct neural strategies across a large repertoire of contractile conditions in different muscles. Our proposed approach may open new avenues for characterizing the relationship between MU firing and twitch properties and their influence on force capacity. This can facilitate the development of targeted rehabilitation strategies tailored to individuals with specific neuromuscular conditions.