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We describe a cobalt(III) complex bearing a phosphinoamine ligand, [Cp*Co(1,2‐Ph2PC6H4NH2)(Cl)]Cl (1), as a proton reduction catalyst which is not only electrochemically active but also delivers good photocatalytic performance. In a system containing semiconductor quantum dots (QDs) and ascorbic acid, complex 1 achieves proton reduction, producing H2 with a turnover number >10000 and an apparent quantum yield of 5.51 % at 450 nm. The important role of the nitrogen basic site in the cobalt first coordination sphere is demonstrated by the difference in the reactivity of two cobalt complexes 1 and [Cp*Co(1,2‐Ph2PC6H4N(Me)2)(Cl)]Cl (2), in which the latter, with a tertiary amine leads to a lower turnover number of circa 6000 for proton reduction. [ABSTRACT FROM AUTHOR]