Several amino acid-based photo-active monomeric iron(III) complexes of the general formula,[Fe(L)₂]PP^-, where L= Schiff base ligands (salisalidene arginine, salicylidenetryptophan, 3,5-di-tert-butyl benzalidine arginine and salicylidene tryptophan) were synthesized, characterized and explored for photoactivated anticancer activity to Chang Liver Cells, HeLa and MCF-7 cells. Complexes exhibited remarkable photo-cytotoxicity with IC₅₀ value to the extent of 0.7 μM to Chang Liver Cells in visible light and there wasa 40-fold enhancement in cytotoxicity in comparison to the cytotoxicity in dark. Complexes were non-toxic to MCF-10A (normal cells) in dark and visible light (IC₅₀ > 100 μM in dark; IC₅₀ > 80 μM in visible light) signifying target-specific nature of the anti-tumour activity of the complexes. Increased ROS concentration,as probed by DCFDA assay, in the cancer cells was responsible for apoptotic cell death. Decarboxylation or phenolate-Fe(III) charge transfer of photo-activated iron(III) complexes generating • OH radicals (ROS) were responsible for the apoptosis. Overall, the tumour-selective photo-activated anticancer activity of the amino acidbased iron(III) complexes have shown a promising aspect in developing iron-based photo-chemotherapeutics as the next generation PDT agents.