The controllable and efficient electrochemical preparation of highly crystalline graphene quantum dots (GQDs) in an aqueous system is still challenging. Here, we developed a weak electrolyte-based (typically an ammonia solution) electrochemical method to enhance the oxidation and cutting process and therefore achieve a high yield of GQDs. The yield of GQDs (3-8 nm) is 28%, approximately 28 times higher than the yield of GQDs prepared by other strong electrolytes. The whole preparation process can be accomplished within 2 h because of the effective free radical oxidation process and the suppressed intercalation-induced exfoliation in weakly ionized aqueous electrolytes. The GQDs also showed excellent crystallinity which is obviously better than the crystallinity of GQDs obtained via bottom-up approaches. Moreover, amino-functionalization of GQDs can be realized by manipulating the electrolyte concentration. We further demonstrate that the proposed method can also be expanded to other weak electrolytes (such as HF and H2S) and different anode precursor materials (such as graphene/graphite papers, carbon fibers, and carbon nanotubes).