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In this study, we propose composite materials based on the Li–Mn–Ti–O system to develop low cost and environmentally benign cathode materials for Li-ion batteries. Specifically, spinel-layered Li2MnTiO4+z (0.5LiMnTiO4•0.5Li2Mn0·5Ti0·5O3) material is studied with the aim to increase the operating voltage of the cathode. In contrast, to increase the capacity as well as rate capability of the cathode, an electrospinning technique is employed to synthesize uniform nanofibers with diameters of approximately 80 nm and a length of 15 μm. The hetero- and one-dimensional structure of the prepared sample facilitate Li+ transport by shortening the diffusion length for the ions. Consequently, high capacities of 210 (average operating voltage ~3.1 V) and 150 mAh g−1 at C/10 and 1C rates, respectively, are obtained.