Abstract Metal‐complex‐based materials for lithium storage have attracted great interest due to their highly designable structures with multiple active sites and well‐defined lithium transport pathways. Their cycling and rate performances, however, are still constrained by structural stability and electrical conductivity. Herein, we present two hydrogen‐bonded complex‐based frameworks with excellent lithium storage capability. Multiple hydrogen bonds among the mononuclear molecules result in three‐dimensional frameworks that are stable in electrolyte. The origin of the remarkable lithium storage performance of this family was revealed through kinetic analysis and DFT calculations.