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Defects engineering is significant for photocatalytic environment remediation. To this end, visible‐light‐driven α‐Fe2O3/ZrO2‐x S‐scheme heterojunction photocatalysts with optimal oxygen vacancy (Ov) defects are successfully synthesized via a two‐step method. Compared with pristine UiO‐66‐NH2‐derived ZrO2‐x and α‐Fe2O3, the heterojunction photocatalysts exhibit a wider range of visible light response and higher efficiency in separating photogenerated electron–hole pairs. Among them, the 5% α‐Fe2O3/ZrO2‐x sample shows the best photocatalytic performance to the degradation of tetracycline (TC) (89.3%), in which the pseudo‐first‐order kinetic rate constants are 8.20 and 16.75 times that of pristine ZrO2‐x and α‐Fe2O3, respectively. The outstanding photocatalytic degradation efficiency can be attributed to both the narrow‐bandgap ZrO2‐x with visible light response and the formation of α‐Fe2O3/ZrO2‐x S‐scheme heterojunctions. During the formation of heterojunctions, the concentration of oxygen vacancies (Ov) at the interface of α‐Fe2O3/ZrO2‐xdecreases monotonically with the increasing loading of α‐Fe2O3, thereby altering the electronic structure of the photocatalyst and forming the heterojunction firmly. In addition, the high stability implies the potential applications in fields of environment. [ABSTRACT FROM AUTHOR]