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Low utilization of solar energy remains a challenge that limits photocatalytic efficiency. To address this issue, this work proposes a bionic solar photocatalytic reactor (BSPR) for efficient selective oxidation of aromatic alcohols. A biomimetic phototropic hydrogel is prepared by coupling chlorine‐doped polypyrrole (Cl‐PPy) and poly(N‐isopropyl acrylamide) (PNIPAm) to maximize light‐harvesting efficiency automatically, allowing the BSPR to maintain high catalytic levels throughout the day. Molecular dynamics simulations are used to unveil the understanding of the fast photoresponsive behavior of Cl‐PPy/PNIPAm from a molecular level, while COMSOL simulations are conducted to follow the macroscopically phototropic mechanism of BSPR. Attributing to the existence of PdS/S vacancies riched ZnIn2S4 nanocomposite in the top flower‐shaped hydrogel, the BSPR displays a special function for efficiently photocatalytic oxidation of aromatic alcohols under solar illumination (yield of 4‐methoxybenzaldehyde: 479.5 µmol g−1 h−1; selectivity: 68.8%). Two possible reaction pathways are identified as follows: photogenerated holes can attract aromatic alcohols directly and generate aromatic aldehydes; photoexcited electrons oxidize O2 to ·O2− can also react with the adsorbed aromatic alcohol. This study presents a promising paradigm that explores opportunities for enhanced utilization of light energy, offering a novel approach to maximize its efficiency in practical applications. [ABSTRACT FROM AUTHOR]