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[Display omitted] • Introduction of spinel-layered Li 3 MnTiO 4+ z cathode materials. • Heterostructure of the cathode material enables facile Li+ transport. • Activation of the layered phase increases voltage and capacity of the cathode. Herein, a layered-spinel structure of Li 3 MnTiO 4+ z (0.8Li 2 Mn 0.5 Ti 0.5 O 3 •0.2LiMnTiO 4) as a working electrode (WE) for Li-ion batteries was synthesized successfully by a solid-state reaction. The cathode delivers a capacity of 80 mAh g−1 for the first discharge. During a working cycle of the battery, the layered-phase material was activated, which contributes to the voltage increase in the 3 V region. The layered phase activation also contributes to the rise in cathode capacity and after 24 cycles, it could reach a capacity of 190 mAh g−1. Moreover, numerous Ti atoms substituted for Mn, and the composite structure facilitated the fast Li+ diffusion, leading to the Li+ diffusion coefficient number in the cathode showing a high value of 3.28 × 10−10 cm2 s−1. [ABSTRACT FROM AUTHOR]