s: The titanium dioxide (TiO2; anatase as main phase) nanoparticles were prepared by the homogenous precipitation, using ammonium titanium oxalate ((NH4)2TiO(C2O4)2•H2O) and urea (CO(NH2)2) as precipitant, followed by the heat treatment in air. The preparation of the fibrous octacalcium phosphate (Ca8(HPO4)2(PO4)4•5H2O: OCP) was also conducted by homogeneous precipitation. The homogeneous mixing of TiO2 nanoparticles with fibrous OCP was conducted by suction filtration, and the hybridized sheet was obtained by the heat treatment in air. Although OCP was thermally decomposed to form hydroxyapatite (Ca10(PO4)6(OH)2) and γ-calcium diphosphate (γ-Ca2P2O7), the fibrous morphology remained unchanged. The TiO2 nanoparticles were homogeneously dispersed on the surface of fibrous OCP. The excellent photocatalytic performance of the hybridized sheet was confirmed by the rapid degradation of the methylene-blue solution. Overall, TiO2-OCP hybridized sheets were found to possess potential utilization in the field of environmental remediation and wastewater treatment.