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Dimension and solvent molecules affect the performance of energetic metal–organic frameworks (EMOFs). High-dimensional EMOFs are usually characterized by high stability and low sensitivity due to their complex network structure. However, solvent molecules affect the detonation performance of EMOFs, and these molecules may be removed at low temperatures, resulting in structural collapse and affecting the stability of EMOFs. In this work, zero-dimensional (0D) Co(AFTO)2·(H2O)2(EMOF 1) and Ni(AFTO)2·(H2O)2(EMOF 2) with coordinated water molecules and [Co(AFTO)2]n·EtOH (EMOF 3) and [Ni(AFTO)2]n(EMOF 4) (AFTO = 5-(4-amino-furazan-3-yl)-1-hydroxytetrazole) with high-dimensional structure were synthesized using hydrothermal and self-assembly methods in ethanol, respectively. Structural and performance tests show that EMOF 3and 4exhibit remarkable thermal stability and low mechanical sensitivity. This method is a simple, effective, and green technique for synthesizing high-dimensional EMOFs with high stability through self-assembly in ethanol solution. In addition, EMOF 3and 4can be used as primary green laser explosives.