This study presents a novel strategy to melt-quench the formation of glasses from a family of metal-carboxylate frameworks (MCFs), which are a significant subclass of metal-organic frameworks (MOFs). By grafting zwitterions onto the carboxylate ligands and incorporating organic acids into the framework channels, the charge delocalization and increased structural disorder facilitate the coordination bonding mismatch, reducing the melting temperature. This approach successfully enables the glass formation of UiO-67, UiO-68, and DUT-5, which are typically considered unmeltable due to their high coordination numbers and large porosity. The resulting glasses exhibit improved thermal stability and processability compared to their crystalline counterparts, opening up new avenues for the development of MOFs with enhanced properties for various applications.This study presents a novel strategy to melt-quench the formation of glasses from a family of metal-carboxylate frameworks (MCFs), which are a significant subclass of metal-organic frameworks (MOFs). By grafting zwitterions onto the carboxylate ligands and incorporating organic acids into the framework channels, the charge delocalization and increased structural disorder facilitate the coordination bonding mismatch, reducing the melting temperature. This approach successfully enables the glass formation of UiO-67, UiO-68, and DUT-5, which are typically considered unmeltable due to their high coordination numbers and large porosity. The resulting glasses exhibit improved thermal stability and processability compared to their crystalline counterparts, opening up new avenues for the development of MOFs with enhanced properties for various applications.