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The search for stable alternative lead-free perovskites has identified all-inorganic antimony/bismuth halide derivatives as promising materials. Despite attractive optoelectronic properties, their wider band gaps and poor morphological control have greatly limited their solar device performance. In this study, we used the indacenodithiophene-based organic acceptor (ITIC) as a Lewis base to improve the morphology of Cs3Sb2I9 films and also as an electron transport layer to form a complimentary heterojunction, and, thereby, enhance the performance of Cs3Sb2I9 solar cells. The presence of cyano and carbonyl groups in ITIC modulated the rate of crystallization of Cs3Sb2I9 and improved its optoelectronic properties. The panchromatic absorption of the Cs3Sb2I9/ITIC heterostructure provided a power conversion efficiency of 3.25% in inverted solar cell structure under 1-sun irradiation. This enhanced performance when using a complimentary absorption strategy suggests a new pathway for developing wider-band-gap lead-free perovskite derivatives for solar cell applications. Moreover, the optimized Cs3Sb2I9/ITIC heterostructure–based solar cell achieved a PCE of 9.2% under indoor illumination at 1000 lx, highlighting the potential use of such devices in indoor applications.