A new Y-based metal–organic framework (MOF) GR-MOF-6 with a chemical formula of {YL­(DMF)2·(DMF)} n {H3L = 5-(4-carboxyphenyl)­ethynyl isophthalic acid; DMF = N,N-dimethylformamide} has been prepared by a solvothermal route. Structural characterization reveals that this novel material is a three-dimensional MOF in which the coordination of the tritopic ligand to Y­(III) metal ions leads to an intercrossing channel system extending over three dimensions. This material has proven to be a very efficient catalyst in the cyanosilylation of carbonyls, ranking second in catalytic activity among the reported rare earth metal-based MOFs described so far but with the lowest required catalyst loading. In addition, its electrophoretic behavior has been studied in depth, providing a zero-charge point between pH 4 and 5, a peak electrophoretic mobility of −1.553 μm cm V–1 s–1, and a ζ potential of −19.8 mV at pH 10.