Spinel-layered composites of Li1.5MnTiO4+δ were studied for their use as high-energy, low-cost, and environmentally benign cathode materials. The bulk particles showed an attractive specific capacity of up to 250 mAh g−1 at C/10. To improve the performance of this cathode at a high C-rate, a spinel-layered Li1.5MnTiO4+δ nanorod was successfully synthesized using a β-MnO2 nanorod template. The nanorod, which had an average diameter of 200 nm and a length of 1 μm, showed specific capacity as high as the bulk particle at C/10. However, owing to a one-dimensional nanostructure with a large effective contact area for Li+ diffusion, the nanorod sample exhibited enhanced capacities 11% (170 mAh g−1) and 167% higher (80 mAh g−1) at 1C and 10C rates, respectively, compared to the bulk particles. Moreover, both samples showed good cycle stability and capacity retention of over 85% after 100 cycles at 1C.