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Photocatalytic oxygen reductive H2O2 production is a promising approach to alternative industrial anthraquinone processes while suffering from the requirement of pure O2 feedstock for practical application. Herein, we report a spaced double hydrogen bond (IC−H‐bond) through multi‐component Radziszewski reaction in an imidazole poly‐ionic‐liquid composite (SI‐PIL‐TiO2) and levofloxacin hydrochloride (LEV) electron donor for highly efficient and selective photocatalytic air reductive H2O2 production. It is found that the IC−H‐bond formed by spaced imino (−NH−) group of SI‐PIL‐TiO2 and carbonyl (−C=O) group of LEV can switch the imidazole active sites characteristic from a covered state to a fully exposed one to shield the strong adsorption of electron donor and N2 in the air, and propel an intenser positive potential and more efficient orbitals binding patterns of SI‐PIL‐TiO2 surface to establish competitive active sites for selectivity O2 chemisorption. Moreover, the high electron enrichment of imidazole as an active site for the 2e− oxygen reduction ensures the rapid reduction of O2. Therefore, the IC−H‐bond enables a total O2 utilization and conversion efficiency of 94.8 % from direct photocatalytic air reduction, achieving a H2O2 production rate of 1518 μmol/g/h that is 16 and 23 times compared to poly‐ionic‐liquid composite without spaced imino groups (PIL‐TiO2) and TiO2, respectively. [ABSTRACT FROM AUTHOR]