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The photoinduced electron-transfer reactions in a Mn₂^II,II−Ru^II−NDI triad (1) ([Mn₂(bpmp)(OAc)₂]⁺, bpmp = 2,6-bis[bis(2-pyridylmethyl)aminomethyl]-4-methylphenolate and OAc = acetate, Ru^II = tris-bipyridine ruthenium(II), and NDI = naphthalenediimide) have been studied by time-resolved optical and EPR spectroscopy. Complex 1 is the first synthetically linked electron donor−sensitizer−acceptor triad in which a manganese complex plays the role of the donor. EPR spectroscopy was used to directly demonstrate the light induced formation of both products:  the oxidized manganese dimer complex (Mn₂^II,III) and the reduced naphthalenediimide (NDI^•-) acceptor moieties, while optical spectroscopy was used to follow the kinetic evolution of the [Ru(bpy)₃]²⁺ intermediate states and the NDI^•- radical in a wide temperature range. The average lifetime of the NDI^•- radical is ca. 600 μs at room temperature, which is at …