Finally, based on the performed simulations and experiments, we propose a melting mechanism of the Co(hmba)3[CoBr4] system with and without water addition, which is expected to also apply to other transition metal-based bis-acetamide hybrid coordination networks. First, upon heating of the anhydrous system, the labile bonds between Co and O in hmba (i.e., the red spheres in Figure ) tend to break, leading to a decrease in the overall network connectivity and ultimately the formation of a molten state. This is accompanied by minor breakage of the tetrahedral [CoBr4] 2- units. Upon cooling this liquid into the solid glass state, the [CoBr4] 2-units reform, while the Co-O network undergoes partial reformation (Figure ). By addition of water to the crystal, the temperature-induced de-coordination process is dramatically enhanced.