Polysulfone (PSF) medical waste can be effectively repurposed due to its excellent mechanical properties. Due to the increasing need for load-bearing bone implants, it is crucial to prioritize the development of biocompatible polymer–matrix composites. Calcium silicate (CaSi), known for its osteogenesis and antibacterial properties, is widely used in medical applications. In this study, recycled PSF plastics in fiber or nanoparticle forms and commercial PSF products were used to create PSF-based composites filled with three different amounts (10, 20, and 30 vol%) of CaSi. The green compact was heat-treated at various temperatures. Experimental results showed that the mechanical interlocking of the PSF matrix and CaSi filler occurred due to the liquefaction of PSF fibers or nanoparticles during heat treatment. When the composite contained 20% CaSi, the obtained three-point bending strength exceeded 60 MPa, falling within the reported strength of compact bone. There was a concurrent improvement in the biocompatibility and antibacterial activity of the PSF-based composites with the increasing amount of CaSi. Considering their mechanical properties and antibacterial activity, the 20% CaSi-containing PSF-based composites treated at 240 °C emerged as a promising candidate for bone implant applications. This study demonstrated the feasibility of upcycling medical waste such as PSF as a matrix, opening doors for its potential usage in the medical field.