Carbon-based materials based on structural and dimensional optimization are appealing as anode materials in lithium-ion batteries (LIBs). However rational design of high-efficiency low-dimensional carbon-based electrodes is still challenging. Therefore, a synthesis strategy based on Schiff base reaction has been devised for S, N co-doped and surface-enriched concave pores coupled with two-dimensional lotus-leaf-like carbon nanosheets (S, N-SCP/LCN). Experimental and theoretical results disclose that the synergetic effect of S, N co-doping and surface concave pores synergistically contribute to the improved lithium storage efficiency. The numerous concave pores within the defective carbon substrates significantly enhance the specific surface area and boost the quantity of active sites. Furthermore, S, N co-doping induces additional surface and structural defects and widens the crystallographic spacing. Herein, the formed threefold lithium storage mechanisms work synergistically to increase the active lithium storage sites and ion diffusion channels, promoting ion diffusion and charge transfer during lithium storage. As expected, the S, N-SCP/LCN exhibits remarkably high lithium storage capacity (1250 mAh/g at 0.1 A/g) and exceptional rate performance (445.65 mAh/g at a high rate of 10 A/g).