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Three-dimensional (3D) urchin-like zinc oxide (ZnO)/titanium dioxide (TiO 2) composite micronanostructures were first successfully synthesised using a facile electrochemical deposition method by depositing TiO 2 into the surface of as-prepared 3D urchin-like ZnO, and polydienes dimethylammonium chloride as polycation solution. Photoelectric properties of the single 3D urchin-like ZnO and the composite micronanostructures as dye-sensitised solar cell (DSSC) anodes were investigated. During the deposition reaction, the TiO 2 was exactly densely anchored onto the surface of 3D urchin-like ZnO with uniform size, which were characterised by scanning electron microscopy, X-ray diffraction, and energy dispersive X-ray spectroscopy. The effects of different molar ratios of TiO 2 and ZnO for the composite structure's morphology and photocatalytic activity were investigated systematically. The results indicated that the composite micronanostructures exhibited a larger adsorption range (−450 nm) and higher photoelectric conversion efficiency due to the synergistic effects, planar heterojunction, and mesoporous structure. When used as photoanodes for DSSCs, the I-V curve showed the photoelectric conversion efficiency of the novel composite was increased by 17.7% of that compared with the single 3D urchin-like ZnO. These features collectively demonstrated the composite has a considerable potential for various applications in photocatalysis materials.