Growing age and different conditions often require the replacement of orthoses, and FDM-based 3D printing can produce them quickly with less investment. In today’s market for orthotics, these characteristics are highly desired. Therefore, this study is fully focused on the optimization and strength analysis of FDM 3D-printed ankle–foot orthoses (AFO) fabricated using PLA and PLA reinforced with carbon fiber (PLA-C). An increase in ankle plantar-flexor force can be achieved by reinforcing thermoplastic AFOs with CFs. Specially designed mechanical strength tests were conducted at the UTM to generate force–displacement curves for stored elastic energy and fracture studies. The mechanical behavior of both AFOs was predicted with the help of an FEA. The model predictions were validated by comparing them with mechanical strength testing conducted under the same loading and boundary conditions as the FEA. In both the prediction and experimental analysis, the PLA-C-based AFOs were stiffer and could withstand greater loads than the PLA-based AFOs. An area of high stress in the simulation and a fracture point in experimentation were both found at the same location. Furthermore, these highly accurate models will allow the fabrication of AFOs to be improved without investing time and resources on trials.