Owing to high safety, low cost, nontoxicity, and environment-friendly features, LiFePO4 that is served as the lithium ion battery cathode has attracted much attention. In this paper, a novel 3D LiFePO4@C core-shell configuration anchored on carbon cloth is synthesized by a facile impregnation sol-gel approach. Through the binder-free structure, the active materials can be directly combined with the current collector to avoid the falling of active materials and achieve the high-efficiency lithium ion and electron transfer. The traditional slurry-casting technique is applicable for pasting LiFePO4@C powders onto the 2D aluminum foil current collector (LFP-Al). By contrast, LFP-CC exhibits a reversible specific capacity of 140 mAh·g-1 and 93.3 mAh·g-1 at 1C and 10C, respectively. After 500 cycles, no obvious capacity decay can be observed at 10C while keeping the coulombic efficiency above 98%. Because of its excellent capacity, high-rate performance, stable electrochemical performance, and good flexibility, this material has great potentials of developing the next-generation high-rate performance lithium ion battery and preparing the binder-free flexible cathode. © 2020 Boqiao Li et al.