For lithium ion batteries, fast charging technology is one of the most important research topics in current society. Transition metal oxides show broad application prospects due to their obvious pseudocapacitive effect. We choose Fe3O4 as the template to design the enhanced pseudocapacitance effect considering of its high theoretical specific capacity and superior structural adjustability. The nanohybrid materials with multiple ionically bonded interfaces accumulated the giant pseudocapacitive effect to obtain superior specific capacity. As a result, the nanohybrid shows a ranking specific capacity over 800 mAh g−1 at 1 A g−1 for 1000 cycles as well as excellent rate capabilities. The existence of interfacial pseudocapacitive effect was confirmed by the kinetic analysis calculating from CV curves. Furthermore, the computation simulation based on the density functional theory (DFT) highly corresponded with our viewpoint about interfacial lithium storage. Our findings pave a novel path for designing novel electrode materials and could further advance the development of lithium-ion batteries with long-term stability and superhigh capacity.