The reaction of [MoH4(depe)2] (1) (depe=1,2‐bis(diethylphosphino)ethane) with different proton sources (HPtBu3+, C6H5COOH, C6F5COOH, H2SO4) was investigated. Whereas complete conversion of 1 into its protonated form is observed in the presence of the phosphonium salt, [MoH5(depe)2]+ only transiently forms upon treatment with the other acids. Further reactivity of the pentahydride complex is indeed noticed with the conjugated base, typically resulting in the formation of neutral (C6F5COOH, H2SO4) or cationic (PhCOOH) molybdenum dihydride complexes. The compounds were characterized by NMR spectroscopy and X‐ray crystallographic studies were performed when suitable crystals were obtained.