Due to its inherent properties and wide availability, cellulose acetate is an extremely competitive candidate for the production of polymeric membranes. However, for best results in particular applications, membrane modification is required in order to minimize unwanted interactions and introduce novel characteristics to the pristine polymer. In this study, the surface of commercial cellulose acetate membranes was functionalized with 4'-aminobenzo-15-crown-5 ether, using a covalent bonding approach. The main goal was the improvement of the membranes biomineralization ability, thus making them prospective materials for bone regeneration applications. The proposed reaction mechanism was confirmed by XPS and NMR analysis while the presence of the functionalization agents in the membranes structure was showed by ATR FT-IR and Raman spectra. The effects of the functionalization process on the morphology, thermal and mechanical properties of the membranes were studied by SEM, TGA and tensile tests. The obtained results revealed that the cellulose acetate membranes were successfully functionalized with crown ether and provided a good understanding of the interactions that took place between the polymer and the functionalization agents. Moreover, promising results were obtained during the Taguchi biomineralization studies. SEM images, EDX mapping and XRD spectra indicating that the CA-AB15C5 membranes have a superior Ca2+ ions retention ability, this causing an accentuated calcium phosphate deposition on the modified polymeric fibers, compared to the neat CA membrane.