The copper and gold metal-organic frameworks (MOFs) [Cu(3)(BTC)(2)(H(2)O)(3)](n), [Cu(3)(BTC)(2)] (BTC=benzene-1,3,5-tricarboxylate), and IRMOF-3-SI-Au are active and reusable solid catalysts for the cyclopropanation of alkenes with high chemo- and diastereoselectivities. This type of material gives better results than previous solid catalysts while working together with the homogeneous catalysts. These MOFs can help to bridge the gap between homogeneous and heterogeneous catalysis.