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Antimony (Sb) demonstrates ascendant reactive activation with lithium ions thanks to its distinctive puckered layer structure. Compared with graphite, Sb can reach a considerable theoretical specific capacity of 660 mAh g⁻¹ by constituting Li₃Sb safer reaction potential. Hereupon, with a self-supported organic carbon as a three-dimensional polymer network structure, Sb/carbon (3DPNS-Sb/C) composites were produced through a hydrothermal reaction channel followed by a heat disposal operation. The unique structure shows uniformitarian Sb nanoparticles wrapped in a self-supported organic carbon, alleviating the volume extension of innermost Sb alloying, and conducive to the integrality of the construction. When used as anodes for lithium-ion batteries (LIBs), 3DPNS-Sb/C exhibits a high invertible specific capacity of 511.5 mAh g⁻¹ at a current density of 0.5 A g⁻¹ after 100 cycles and a remarkable rate property of 289.5 mAh g⁻¹ at a current density of 10 A g⁻¹. As anodes, LIBs demonstrate exceptional electrochemical performance.