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Halide perovskites with low-dimensionalities (2D or quasi-2D) have demonstrated outstanding stabilities compared to their 3D counterparts. Nevertheless, poor charge-transporting abilities of organic components in 2D perovskites lead to relatively low power conversion efficiency (PCE) and thus limit their applications in photovoltaics. Here, we report a novel hole-transporting low-dimensional (HT2D) perovskite, which can form a hole-transporting channel on the top surface of 3D perovskite due to self-assembly effects of metal halide frameworks. This HT2D perovskite can significantly reduce interface trap densities and enhance hole-extracting abilities of a heterojunction region between the 3D perovskite and hole-transporting layer. Furthermore, the posttreatment by HT2D can also reduce the crystal defects of perovskite and improve film morphology. As a result, perovskite solar cells (PSCs) can effectively suppress nonradiative recombination, leading to an increasement on photovoltage to >1.20 V and thus achieving >20% power conversion efficiency and >500 h continuous illumination stability. This work provides a pathway to overcome charge-transporting limitations in low-dimensional perovskites and delivers significant enhancements on performance of PSCs.