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To solve the problem associated with the huge volume change and low conductivity of Mn3O4, a novel C/Mn3O4microsphere with Mn3O4layer and void space sandwiched by nitrogen‐doped carbon (NC) is designed and fabricated. In this composite, the NC is obtained from the metal–organic frameworks (MOFs) and polydopamine (PDA). The preparation process is facile and effective without additional templates or redox solvents introduced. When used as anodes for lithium‐ion batteries (LIBs), the C/Mn3O4composite incorporates the metrics of N‐doping, yolk‐shell structure, double carbon layer, mesoporous Mn3O4, showing an outstanding lithium storage of ≈1015.9 mAh g−1at 0.2 A g−1in the 250th cycle, high cycling stability (without clear capacity decay after 400 cycles), and excellent rate capability (capacity can fully recover as the current density returns back to the initial value of 0.2 A g−1). The yolk‐shell structure derived from MOFs can be expanded to fabricate other materials with improved performance. A novel C/Mn3O4microsphere with Mn3O4layer and void space sandwiched by N‐doped carbon (NC) layers (derived from metal–organic frameworks or polydopamine) is synthesized via hydrothermal technique and heat treatment. The synthesis process is facile and effective without additional templates or redox solvents introduced. Incorporating the merits of mesoporous Mn3O4, NC, and yolk‐shell structure, the C/Mn3O4electrodes show high electrochemical performance.