Authors have synthesized a novel yttrium-pillared silicotungstate dimer by the reaction of TBA4H4[ホウ-SiW10O36] (SiW10) with Y(acac)3 in an org. medium (acetone). In the presence of TBA8H2[(ホウ-SiYW10O36)2]ツキ7H2O (Y2), cyanosilylation of several structurally diverse ketones and aldehydes with TMSCN selectively proceeded to afford the corresponding cyanohydrin trimethylsilyl ethers. In particular, the catalytic performance for aldehydes was very significant; for example, TON = 18000 and TOF = 540000 h-1 were obsd. for n-hexanal. [on SciFinder(R)]