A new porous metal-organic framework (MOF) with the chemical formula Y 5 L 6 (OH) 3 (DMF) 3 ·5H 2 O ( 1 ) (where L = 3-amino-4-hydroxybenzoate) has been prepared by a solvothermal procedure. The structural characterization reveals that this material consists of a robust three-dimensional metal-organic framework (MOF) grown with clusters formed by Y( iii ) and hydroxide anions joined to one another by the ligand, giving rise to an open structure with interconnected microchannels with variable dimensions. This assembled set has shown to possess a fascinating catalytic activity for the cyanosilylation of a broad range of aldehydes and ketones with exceptional recyclability, a solvent-free medium, and one order of magnitude lower catalyst loading compared to all related lanthanide-based MOFs described so far in the literature. A novel MOF has been synthesized, characterized, and applied in the cyanosilylation of aldehydes and ketones being the first example of an yttrium MOF able to catalyze this reaction.