Sustainable assembly of imidazolidines is accomplished via a sequential stereospecific ring opening and C-H amination using aziridines with secondary cyclic amines under visible light mediated indazoloquinoline photoredox catalysis at ambient conditions. Optically active aziridines are coupled with high enantiomeric purities. The computational studies provide insights on the redox properties of the catalysts as well as a profile of the reaction.