A honeycomb‐like 3D N/S co‐doped porous carbon‐coated cobalt sulfide (CoS, Co9S8, and Co1–
xS) composite (CS@PC) is successfully prepared using polyacrylonitrile (PAN) as the nitrogen‐containing carbon source through a facile solvothermal method and subsequent in situ conversion. As an anode for lithium‐ion batteries (LIBs), the CS@PC composite exhibits excellent electrochemical performance, including high reversible capacity, good rate capability, and cyclic stability. The composite electrode delivers specific capacities of 781.2 and 466.0 mAh g−1 at 0.1 and 5 A g−1, respectively. When cycled at a current density of 1 A g−1, it displays a high reversible capacity of 717.0 mAh g−1 after 500 cycles. The ability to provide this level of performance is attributed to the unique 3D multi‐level porous architecture with large electrode–electrolyte contact area, bicontinuous electron/ion transport pathways, and attractive structure stability. Such micro‐/nanoscale design and engineering strategies may also be used to explore other nanocomposites to boost their energy storage performance.