It is a significant challenge to construct chiral metal-organic frameworks (CMOFs) by developing a facile and green preparation strategy. In this work, CMOFs were first synthesized via a mechanochemical process by combining a truncated mixed ligand strategy and defect engineering theory. The simple, green, and rapid construction strategy could solvent-freely harvest gram-scale CMOFs with a hierarchical micro/mesoporous structure. The as-synthesized CMOFs were evaluated by Aldol asymmetric catalysis and exhibited excellent catalytic performance (conversion was up to 97.1%, the ee value was 44.3%, and the activity was still good after 5 cycles).