The work aims to construct a nano-TiO2/activated carbon composite surface with excellent purification performance. The sol-gel template method was used to construct the spherical surface. The paraffin ball was prepared by emulsification method and extruded with the nano-TiO2/activated to form a regular stable spherical surface. The surface microstructure, morphology and phase were detected by SEM, XRD and FTIR. The spherical surface structure was reconstructed and analyzed by spherical X-ray tomography. The purification effect of the samples with different equivalent diameters spherical surfaces on methylene blue was analyzed. The mild treatment process maintained the phase and grain size of the original P25 powder, and interconnected, multi-faceted and multi-pore structure and cluster-like uniform surface could be formed by sol-gel template method. The 3DCT results showed that the composite of activated carbon allowed the sample to form carbon-reinforced TiO2 spherical surfaces of different sizes. The successfully constructed nano-TiO2/activated carbon composite surface could completely degrade methylene blue after 8 cycles of adsorption-catalysis test. The purification of the sample with an average equivalent diameter of 0.67 mm maintained at 100% after a 9-cycle purification reaction. Therefore, the sol-gel template method can construct the of nano-TiO2/activated carbon composite spherical continuous surface. The large pore connection between the spherical surfaces and the composite of activated carbon can promote the mass transfer efficiency and improve the cycle purification performance.