Abstract N‐doped carbons as one of the most prominent anode materials to replace standard graphite exhibit outstanding Li+ storage performance. However, N‐doped carbon anodes still suffer from low N‐doping levels and low initial Coulombic efficiency (ICE). In this study, high N‐doped and low graphitic‐N carbons (LGNCs) with enhanced ICE were synthesized by taking advantage of a denitrification strategy for graphitic carbon nitride (g‐C3N4). In brief, more than 14.5 at% of N from g‐C3N4 (55.1 at% N) was retained by reacting graphitic‐N with lithium, which was subsequently removed. As graphitic‐N is largely responsible for the irreversible capacity, the anode's performance was significantly increased. Compared to general N‐doped carbons with high graphitic‐N proportion (>50%) and low N content (