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The redox non\u2010innocent BPI pincer ligand allows for efficient charge transfer homolytic processes of the title compounds. This makes them a universal platform for the generation of carbon\u2010centered radicals. The photo\u2010induced homolytic cleavage of the Al\u2212C bonds was investigated by means of stationary and transient UV\/Vis spectroscopy, spin trapping experiments, as well as EPR and NMR spectroscopy. The experimental findings were supported by quantum chemical calculations. Reactivity studies enabled the utilization of the aluminum complexes as reactants in tin\u2010free Giese\u2010type reactions and carbonyl alkylations under ambient conditions, which both indicated radical\u2010polar crossover behavior. 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