This study presents two main aims: (i) to assess functionally-calibrated musculoskeletal models (FCMs) in both tracking and predictive simulations of human motion, against non-linearly scaled models (NSMs), and (ii) to examine the effects of three different variations of our baseline functional calibration approach on the results of tracking and predictive simulations. Methods: Motion capture experiments of six functional activities were performed with three healthy subjects. The musculotendon (MT) parameters of 18 muscles per leg were estimated using an optimal control problem. A baseline problem formulation and three variations were developed to generate four different FCMs per subject. Then, the FCMs were compared against NSMs in tracking simulations of the motions excluded from the calibration and fully-predictive simulations of gait. Results: In the tracking simulations, the FCMs led to more accurate joint torques estimations. Including gait in the calibration problems improved the knee torques accuracy (normalised root mean square error: 0.31+/-0.11), compared to the baseline calibration (normalised root mean square error: 0.70+/-0.21). Regarding the gait predictive simulations, the NSMs consistently yielded more accurate subtalar inversion/eversion torques and knee flexion angles, compared to the FCMs. The accuracy of the predicted muscle excitations was generally consistent between NSMs and FCMs. Conclusion: The results suggest that, while the FCMs led to more accurate joint torques estimations in the tracking simulations, they did not outperform the NSMs in the fully-predictive gait simulations.