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An efficient approach has been developed for the enantioselective synthesis of inherently chiral quinoline-fused calix[4]arenes through palladium-catalyzed asymmetric mono-/double C-H cycloimidoylation of isocyano-calix[4]arenes.The cyclization strategy of forming a six-membered heterocyclic ring employs readily available calix[4]arene derived isocyanides and aryl iodides as coupling partners under mild conditions with low catalyst loading, and a wide range of calix[4]arenes with extended aromatic systems were obtained with high yields and excellent enantioselectivities (up to >99% ee).Density functional theory (DFT) calculations reveal the origin of the enantioselectivity during the C(sp 2 )-H imidoylative cyclization process. Band Gap Matching for Minimized Recombination Loss in Efficient Perovskite/Organic Tandem Solar Cells