A hierarchical microstructure constructed with graphitic-carbon-coated Ni3S2 nanoparticles anchored on N-doped mesoporous carbon nanoflakes was fabricated using a nickel-based micro-nano structure as a precursor and polydopamine as a carbon source. By optimizing the microstructure, the obtained Ni3S2/carbon composite compounded with the thickest carbon nanoflakes delivers ultrafast and stable Na-ion storage performance, and can maintain a reversible charge capacity of 372 mA h g-1 at a current density of 5 A g-1 over 250 cycles, and 316 mA h g-1 even at a current density of 20 A g-1 for 2000 cycles. These remarkable electrochemical properties can be attributed to its hierarchical microstructure of graphitic-carbon-coated Ni3S2 particles and N-doped mesoporous carbon nanoflakes, which provide easy accessibility to the electrolyte, fast electron transport and Na+ diffusion, and even relieve the strain caused by the volume expansion upon cycling.