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The synergistic enhancement of energy-release and safety performance is significant for energetic crystals (ECs), such as 3-nitro-1,2,4-triazole-5-one (NTO) and ammonium perchlorate (AP). However, the sluggish energy-release kinetics, high decomposition temperature, and unsatisfied safety performance have plagued the high-efficiency applications of NTO and AP. Herein, graphene oxide (GO) was utilized to ameliorate the physicochemical features and performance characteristics of NTO and AP using a confined crystallization strategy in liquid nitrogen (LN-NTO@GO and LN-AP@GO). Lamellar GO could act as a lubricant, leading to an excellent improvement in mechanical safety performance. Besides, many functional groups in GO could act as building blocks and active sites for the confined crystallization of ECs. Theoretical investigations indicate an interfacial charge mismatch at the GO-EC interface. The asobtained LN-NTO@GO and LN-AP@GO energetic nanocomposites demonstrate promoted exothermic decomposition temperatures of 18.2 and 70.1°C with substantially accelerated kinetics compared with pristine counterparts and samples crystallized naturally. Reasonable interfacial engineering by interfacial charge mismatch between the catalyst and ECs would break new grounds for designing fast energy-release and safe operation of energetic materials.