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In this study, the ultrafine-grained Ti23Zr25Nb-based composites with 45S5 Bioglass and Ag, Cu, or Zn additions were produced by application of the mechanical alloying technique. Additionally, the base Ti23Zr25Nb alloy was electrochemically modified in the two stages of processing: electrochemical etching in the solution of H₃PO₄ and HF followed by electrochemical deposition in Ca(NO₃)₂, (NH₄)₂HPO₄, and HCl. The in vitro cytocompatibility studies were also done with comparison to the commercially pure titanium. The established cell lines of Normal Human Osteoblasts (NHost, CC-2538) and Human Periodontal Ligament Fibroblasts (HPdLF, CC-7049) were used. The culture was conducted among the tested materials. Ultrafine-grained titanium-based composites modified with 45S5 Bioglass and Ag, Cu, or Zn metals have higher biocompatibility than the reference material in the form of a microcrystalline Ti. Proliferation activity was at a stable level with contact with studied materials. In vitro evaluation research showed that the ultrafine-grained Ti23Zr25Nb-based composites with 45S5 Bioglass and Ag, Cu, or Zn additions, with a Young modulus below 50 GPa, can be further used in the biomedical field.