The molecular strontium hydride [(Me(3)TACD)(3)Sr-3(mu(3)-H)(2)][SiPh3] (2) was isolated as the dark red benzene solvate 2 center dot C6H6 in 69% yield from the reaction of [Sr(SiPh3)(2)(thf)(3)] (1') with (Me(3)TACD)H (1,4,7-trimethyl-1,4,7,10-tetraazacyclododecane). This reaction can be considered as a redox process, with the Bronsted acidic amine proton in (Me(3)TACD)H transformed into the hydride by the anion [SiPh3](-). Trace amounts of water resulted in the formation of [(Me(3)TACD)(3)Sr-3(mu(3)-H)(mu(3)-OH)][SiPh3] (2*), which cocrystallized with 2. Single-crystal X-ray diffraction of 2 revealed a substitutional disorder of a bridging hydride with a hydroxide ligand. Hydride complex 2 was also obtained by hydrogenolysis of [(Me(3)TACD)Sr(SiPh3)] (3), although pure 3 proved difficult to isolate. In the presence of a 2-fold excess of (Me(3)TACD)H, the reaction with disilyl 1' gave [(Me(3)TACD)SiPh3] (4). Complex 2 underwent facile H/D exchange with D-2 (1 bar), with the anion [SiPh3]- decomposing concurrently. In the reaction of 2 with 1,1-diphenylethylene (DPE), the anion [SiPh3](-) was added to the C-C bond in DPE to give [(Me(3)TACD)(3)Sr3H2][Ph2CCH2SiPh3] (5), whereas the cationic cluster [(Me(3)TACD)(3)Sr3H2](+) remained unchanged. 9-Fluorenone underwent one-electron reduction with 2 to give the paramagnetic ketyl complex [{(Me(3)TACD)H}Sr(OC13H8 center dot)(2)(thf)(2)] (6). These strontium compounds are structurally similar to the lighter calcium congeners, but more reactive, in particular with regard to fast H/D exchange and [SiPh3]- anion decomposition. DFT studies on the cationic hydride clusters suggest a more pronounced covalent character for strontium compared to calcium. Disilyl 1, strontium diketyl 6, and the calcium congener of 6, [{(Me(3)TACD)H}Ca(OC13H8 center dot)(2)] (10), were also characterized by X-ray diffraction.