Engineering the structure and increasing the near-surface reaction of carbon materials can show unexpected effects for designing high-rate capability of lithium, sodium-ion batteries (LIBs, SIBs). The edge heteroatom-doping strategy of carbon materials can significantly enhance the Li+ and Na+ adsorption energy. However, achieving ultrahigh content of edge heteroatoms doping is still a great challenge due to the difficulty in tailoring the heteroatom dopant construction. Herein, a facile synthesis method was proposed to design the ultrahigh content of edge nitrogen/oxide/sulfur doping turbostratic carbon (NOS-TC) materials for high-performance LIBs and SIBs. The prepared NOS-TC800 has a 3D microstructure, a large defect spacing, and an ultrahigh content (21.70 at%) of edge-N, O, S tri-doping. The NOS-TC800 anode displays a high-rate capability, and accompanied by an ultralong cycling life (214.9 mAh g − 1 after 3500 cycles at 10 A g − 1 in LIBs, 159.6 mAh g − 1 after 3000 cycles at 5 A g − 1 in SIBs). The NOS-TC800 anode-based full cell has a high energy density of 212 Wh kg−1 for LIBs and 142 Wh kg−1 for SIBs. The strategy of tailored architecture and high-content edge heteroatom-doping demonstrates that it is promising to achieve high-rate capability and energy density for LIBs and SIBs.