In this study we synthesize a novel mesoporous titanium oxide (TiO2) through calcination of a bioinspired supramolecular assembly of polymeric micelles, based on the thymine‐functionalized homopolymer, poly(4‐vinylbenzyl triazolylmethyl‐methylthymine), complexed with Ti(OH)22+ ions. We characterize thin films of these structures using wide‐angle X‐ray diffraction, small‐angle X‐ray scattering, nitrogen adsorption/desorption isotherms, transmission electron microscope, and scanning electron microscope. This approach is simple, effective, and inexpensive when compared with the synthesis of diblock or triblock copolymers typically required to prepare soft templates. This new mesoporous material exhibits superior photocatalytic activity for the degradation of the organic dye methylene blue almost three times higher than that of bulk TiO2.