Owing to their high strength characteristics, chemical stability, and piezoelectric activity, vinylidene fluoride (VDF) copolymers have become promising materials for creating implants to replace bone tissue defects. However, a significant drawback of these materials is the biological inertness of their surface, which leads to unsatisfactory integration with the patient’s bone tissue. In this study, we propose a single-step approach for immobilizing hydroxyapatite (HAp) on the surface of porous implants made of vinylidene fluoride and tetrafluoroethylene copolymer (P(VDF-TeFE)). This method consists of treating the surface of the product with a mixture of solvents while simultaneously capturing HAp microparticles. Using scanning electron microscopy (SEM) and energy-dispersive spectroscopy (EDS), it was shown that the proposed method preserves the morphology of model implants (pore diameter and printed line thickness) and allows HAp to cover up to 63 ± 14% of their surface, reaching concentrations of calcium and phosphorus up to 6.0 ± 1.3 and 3.6 ± 0.7 at. %, respectively, imparting superhydrophilic properties to them. Optical profilometry revealed that the surface roughness of samples increased by more than seven times as a result of HAp immobilization. X-ray diffraction analysis (XRD) confirmed that the piezoelectric phase of P(VDF-TeFE) is preserved after treatment, as are the compressive strength characteristics of the samples. Hydroxyapatite immobilization significantly improved the adhesion and osteogenic differentiation of multipotent stem cells cultured with P(VDF-TeFE)-based samples. Thus, the proposed method can significantly enhance the biological activity of implants based on the piezoelectric VDF copolymer.