Here we present a systematic investigation of the cyanosilylation of aldehydes with trimethylsilyl cyanide (TMSCN) by using metal-organic frameworks (MOFs) as the catalysts. Four types of thermal stable MOFs (MIL-47 (V), MIL-53 (Al), MIL-101 (Cr), and UiO-66 (Zr)) constructed with the same organic linker, terephthalic acid, were studied, among which MIL-101 (Cr) exhibits the highest catalytic activity. Experimental results revealed that the catalytic activities are in close relation with the types of coordinatively unsaturated metal ions, pore sizes as well as solvents. Using MIL-101 (Cr) as the catalyst, both aliphatic and aromatic aldehydes were efficiently transformed to cyanohydrin trimethylsilyl ether, meanwhile significant size selectivities and electronic effects have also been observed. The solvent-free reaction conditions not only provide a high TON for MOF catalyzed cyanosilylation, but also render current protocol more attractive to industrial applications.