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Li2MnSiO4-based cathode materials possess reasonable work potentials and high theoretical capacities, while the practical energy/power densities are constrained by their inferior kinetics of Li+ diffusion. In this work, the Pmn21-structure Li2FexMn1-xSiO4/C materials were synthesized via a solvothermal method and evaluated as Liion cathode materials, with notable morphological evolutions and tunable crystallographic habits observed after solvothermal process. The Li2Fe0.33Mn0.67SiO4/C material delivers an initial reversible capacity of 250.2 mAh g?1 at 0.1 C (~ 1.51 Li+ insertion/extraction, 1 C=166 mA g?1), excellent high-rate capability (52.2 mAh g?1 at 5 C), and good long-term cyclability (64.6% after 196 cycles at 2 C). The enhanced electrochemical properties are attributed to the boosted ion/electron transports induced by preferred morphological and structural characteristics of Li2Fe0.33Mn0.67SiO4/C.