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Two novel isomeric cocrystals based on CL-20 (2,4,6,8,10,12-hexanitrohexaazaisowurtzitane) and MDNI (1-methyl-dinitroimidazole) isomers including a 1:1 CL-20/2,4-MDNI (1) and a 1:1 CL-20/4,5-MDNI (2) were obtained. These cocrystals have high densities, high predicted detonation properties, and low impact sensitivities with excellent thermal stabilities, for example, 2 (ρ: 1.882 g cm–3; D: 8915 m s–1, P: 35.88 GPa; IS: 11 J) exhibits excellent comprehensive performances. Notably, adopting the isomer as a coformer for constructing energetic cocrystals or even new cocrystal forms and further tuning properties represents a study orientation of explosives that is not yet exploited in the energetic material field.