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Abstract The heterointerface between the contacted organic and inorganic semiconductors critically affects the charge extraction, hence overall performance of organic optoelectronics, especially for organic solar cells (OSCs). Herein, we develop an effective interfacial strategy that simultaneously boosts the chemical, electric, and electronic properties of the organic–inorganic heterointerface of the derived OSCs, through implanting conjugated molecules as self‐assemble monolayers (SAMs) to metal oxide nanoparticles (MO NPs). As results, SAM passivated zinc oxide nanoparticles (ZnO NPs) as electron transport layers (ETLs) not only enable the best performed OSCs containing MO ETLs, but also exhibit the most desirable thickness insensitive features (up to 300 nm). In addition, SAM‐ZnO ETLs help also substantially improving the photostability of the derived OSCs. Overall, this work can be beneficial to the further development of high‐performance and cost‐effective OSCs.