Exploring heterometallic architectures and uncoordinated nitrogen sites in zeolitic imidazole–tetrazole frameworks provides an unconventional route to enhancing electrocatalytic activity. Herein, we report a mechanochemical alloying approach that simultaneously induces metal–metal (Co–Zn) and ligand–ligand (imidazole–tetrazole) mixing to yield an amorphous solid solution, aZn0.5Co0.5ZI0.5T0.5F-8, from pristine ZnZTF-8 and CoZIF-8 under solvent-free conditions in an inert atmosphere (Ar). Subsequ