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• A complex gradient passivation strategy was first proposed for inverted PSCs. • In(SCN 2 H 4) 3 Cl 3 effectively passivates defect states in bulk perovskite layer. • In(SCN 2 H 4) 3 Cl 3 facilitates hole extraction by modulating interface energy level alignment. • The efficiency and stability of inverted PSCs are significantly improved. To address the interfacial and bulk defects and mismatched energy band alignment at perovskite/hole transport layr (HTL) interface in inverted perovskite solar cells (PSCs), here a novel In(SCN 2 H 4) 3 Cl 3 complex diffusion doping strategy was proposed to construct CH 3 NH 3 PbI 3 :In(SCN 2 H 4) 3 Cl 3 composite layer for poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine (PTAA)-based inverted PSCs. The In(tu) 3 Cl 3 effectively promotes the quality of perovskite films with larger perovskite crystal grains and flatter and denser surfaces. Both theoretical and experimental results reveal that the In(SCN 2 H 4) 3 Cl 3 can not only passivate interfacial and bulk defects in perovskite layer, but also form a spatial separation of photogenerated charges through CH 3 NH 3 PbI 3 :In(SCN 2 H 4) 3 Cl 3 heterojunction interface, which effectively decreases the charge recombination and enhances charge separation and transport property in PSCs. Moreover, the In(SCN 2 H 4) 3 Cl 3 optimizes energy band alignment at perovskite/PTAA interface and creates a polarization electric field at the PTAA/In(SCN 2 H 4) 3 Cl 3 interface directing toward PTAA layer, which promotes the hole transfer from the CH 3 NH 3 PbI 3 to the PTAA and increases the open-circuit voltage (V oc). As a consequence, optimized inverted PSCs with CH 3 NH 3 PbI 3 :In(SCN 2 H 4) 3 Cl 3 layer achieve high efficiency of 21.25 % and also show a significantly improved long-term stability under different aging test conditions. Our work provides a valuable guide for designing efficient and stable inverted PSCs. [ABSTRACT FROM AUTHOR]