The reactions of [MIr(CO)3(dppm)2] (M = Rh, Ir; dppm = Ph2PCH2PPh2) with methyl triflate yield [RhIr(CH3)(CO)3(dppm)2] [CF3SO3] and the unusual product of C-H activation of a methyl group [Ir2H(CO)3(mu-CH2)(dppm)2] [CF3SO3], respectively. The reactivities of these species with small molecules such as H-2, CO, C2H4, and PR3 are reported.