Crystalline metal-organic frameworks (MOFs) have garnered escalating attention as a type of functional porous materials and demonstrated their promising applications in gas storage, gas separation, catalysis, and others. Their crystallinity is usually achieved by reversible metal–ligand bond formation under solvothermal conditions, which involve reactions at high temperature for an extended period of time in the presence of an excessive amount of toxic solvents. In this presentation, I will demonstrate how mechanochemistry is leveraged as an alternative yet sustainable approach to preparing MOFs. The solid-state mechanochemical synthesis drives chemical reactions via mechanical forces instead of heat, light, or electricity and avoids both high temperature and solvents. Moreover, I will highlight that mechanochemistry provides a unique access to porous materials that cannot be generated by classical solvothermal reactions.