The novel mu-iminosilyl complexes Ru-2(CO)(4)-(mu-dppm)(mu-SiTol(2))(mu-R'CH=NSiTol(2)) (2) were obtained in high yields during the stoichiometric reactions of a diruthenium complex having Ru-H-Si interactions, {Ru(CO)(2)(SiTol(2)H)}(2)(mu-dppm)(mu-eta(2):eta(2)-H(2)SiTol(2)) (1), with nitriles R'CN (R' = Me, Ph, t-Bu, CH=CH2). The catalytic hydrosilylation of various ketones and imines with dihydrosilanes were achieved using 1 as a catalyst. A novel reaction cycle involving the cooperative functions of the two Ru metals is proposed for the related hydrosilylation of various ketones and imines catalyzed by 1.