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Precise manipulation on surface dimensionality benefits the improvement of efficiency and stability of perovskite solar cells, however, heterogeneity with the presence of substantial atomic‐scale impurities and micro‐wrinkles on perovskite surface that serve as transformation template challenges the formation of homogeneous heterointerface and thus weakens healing efficacy. To address this issue, herein, we propose a dual‐mechano‐chemical strategy is proposed to homogenize the morphologic‐compositional feature of perovskite surface by first polishing superficial nano‐impurities with energetic nanoparticles and then in situ dimensionalizing the defect‐free lattice to form a 2D/3D heterointerface with strengthened contact and homogeneous distribution. With the implement of this strategy, the reconstructed heterointerface not only accelerates charge transfer with minimized interfacial non‐radiative recombination losses, but also protects perovskite lattice from external attack. Consequently, an all‐air‐processed carbon‐based CsPbI2Br solar cell displays enhanced efficiency of 15.29% and elevated performance retention rate under dark storage over 1000 h, high temperature over 500 h as well as persistent operation over 200 h. This work provides a multidimensional surface engineering strategy for high‐efficiency and stable perovskite‐based photoelectric device, benefiting the large‐scale fabrication in the future. A homogeneous and strengthened 2D/3D perovskite heterointerface is realized by idealizing the perovskite surface to eliminate atomic‐scale impurities and micro‐wrinkles. Benefiting from the reinforcement of charge transfer and lattice solidification, an all‐air‐processed carbon‐based all‐inorganic CsPbI2Br device achieves an enhanced efficiency of 15.29% with improved stability, offering a deep insight on dimensionality engineering.