The growth of metal-organic frameworks (MOFs) is most frequently accessed by the direct assembly of metal cations and multitopic ready-to-connect ligands under solvothermal conditions. However, such nonambient conditions are expected to impose a synthetic challenge to incorporate degradable ligands into MOFs. This explains why imine-based MOFs are scarce as the imine motif is usually prone to decompose through hydrolysis. This work not only showcases mechanochemistry as an ambient, sustainable, and high-yield strategy for synthesizing a variety of imine-based MOFs but also achieves the integration of ligand synthesis and MOF growth into a single tandem step. Thus, this work provides straightforward access to imine-based MOFs, a subfamily of historically challenging MOF materials.