A strategy is presented to enable the melt-quenching of metal-carboxylate frameworks (MOFs) into glasses, overcoming the challenge of melting large subclasses of MOFs. By grafting zwitterionic groups on carboxylate ligands and incorporating Brønsted acids in framework channels, the charge delocalization of the zwitterion-acid subsystem and the densely filled channels facilitate coordination bonding mismatch, reducing the melting temperature. This approach allows the glass formation of a family of carboxylate MOFs (UiO-67, UiO-68, and DUT-5), which are typically considered un-meltable. The strategy involves covalently bonding zwitterionic groups on rigid aromatic carboxylate ligands and incorporating Brønsted acids in the framework channels. This reduces porosity and enhances configurational entropy, lowering the glass transition and melting temperatures. The resulting glasses are fully meltable, with melting temperatures above 120°C, and exhibit unique properties such as high proton conductivity and structural recovery upon solvent stimulation. The study demonstrates that the covalently bonded zwitterion-acid subsystem significantly reduces the melting temperature of MOFs, enabling their transformation into glasses. The findings open new avenues for melt-quenching porous molecular solids into glasses, with potential applications in various fields. The research highlights the importance of structural modifications in achieving glass formation of MOFs, which are typically difficult to melt due to their high coordination numbers and strong bonds. The successful glass formation of UiO-67, UiO-68, and DUT-5 demonstrates the feasibility of this strategy for a wide range of MOFs. The study also provides insights into the structural and thermodynamic properties of the resulting glasses, including their amorphous nature, isotropic glassy behavior, and unique proton conductivity. The results indicate that the covalent bonding of zwitterionic groups and Brønsted acids plays a crucial role in enabling the glass formation of MOFs, which is essential for their practical applications. The research contributes to the understanding of the mechanisms underlying the glass formation of MOFs and provides a promising approach for the development of new glassy materials from MOFs.A strategy is presented to enable the melt-quenching of metal-carboxylate frameworks (MOFs) into glasses, overcoming the challenge of melting large subclasses of MOFs. By grafting zwitterionic groups on carboxylate ligands and incorporating Brønsted acids in framework channels, the charge delocalization of the zwitterion-acid subsystem and the densely filled channels facilitate coordination bonding mismatch, reducing the melting temperature. This approach allows the glass formation of a family of carboxylate MOFs (UiO-67, UiO-68, and DUT-5), which are typically considered un-meltable. The strategy involves covalently bonding zwitterionic groups on rigid aromatic carboxylate ligands and incorporating Brønsted acids in the framework channels. This reduces porosity and enhances configurational entropy, lowering the glass transition and melting temperatures. The resulting glasses are fully meltable, with melting temperatures above 120°C, and exhibit unique properties such as high proton conductivity and structural recovery upon solvent stimulation. The study demonstrates that the covalently bonded zwitterion-acid subsystem significantly reduces the melting temperature of MOFs, enabling their transformation into glasses. The findings open new avenues for melt-quenching porous molecular solids into glasses, with potential applications in various fields. The research highlights the importance of structural modifications in achieving glass formation of MOFs, which are typically difficult to melt due to their high coordination numbers and strong bonds. The successful glass formation of UiO-67, UiO-68, and DUT-5 demonstrates the feasibility of this strategy for a wide range of MOFs. The study also provides insights into the structural and thermodynamic properties of the resulting glasses, including their amorphous nature, isotropic glassy behavior, and unique proton conductivity. The results indicate that the covalent bonding of zwitterionic groups and Brønsted acids plays a crucial role in enabling the glass formation of MOFs, which is essential for their practical applications. The research contributes to the understanding of the mechanisms underlying the glass formation of MOFs and provides a promising approach for the development of new glassy materials from MOFs.