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Abstract 2D perovskites are relatively stable but possess poor charge transport compared to 3D perovskites. To boost charge transport, novel 2D perovskites mixed with 3D perovskites are developed, where Pb²⁺are partially substituted by the heterovalent neodymium cations (Nd³⁺) within both 2D and 3D perovskites (termed Nd³⁺‐substituted 2D:3D mixed perovskites. Systematical studies reveal that the Nd³⁺‐substituted 2D:3D mixed perovskites possess larger crystals, superior crystallinity, suppressed non‐radiative charge recombination, and enhanced and balanced charge transport compared to the 2D:3D mixed perovskites. As a result, perovskite photovoltaics based on the Nd³⁺‐substituted 2D:3D mixed perovskites exhibit a power conversion efficiency of 22.11%, a photoresponsibility of over 700 mA W⁻¹, a photodetectivity of 4.29 × 10¹⁴ cm Hz^1/2 W⁻¹, a linear dynamic range of 165 dB at room temperature, and dramatically boosted stability. These results demonstrate that, a facile way is developed to realize high‐performance perovskite photovoltaics through partially heterovalent substituted Pb²⁺by Nd³⁺within 2D:3D mixed perovskites.