The constructing of efficient photocatalysts for environmental remediation has attracted a great deal of attention in recent years. In this paper, Cr /UiO‐66‐NH2 was synthesized by the chromium acetylacetone grafted on UiO‐66‐NH2 directly and UiO‐66‐NH2‐SA‐Cr (anchored on the Schiff base UiO‐66‐NH2‐SA with chemical bonds) was prepared by post‐synthesis method, which both provided such support in degrading tetracycline (TC) and xylenol orange (XO) under visible light. Compared with UiO‐66‐NH2 and Cr /UiO‐66‐NH2, the photocatalytic experiments indicated that UiO‐66‐NH2‐SA‐Cr possessed significant enhanced photocatalytic activity, with 76.5 % of tetracycline (TC) and 71.5 % of xylenol orange (XO) being removed under the optimization of experimental conditions. The enhanced photocatalytic activity of UiO‐66‐NH2‐SA‐Cr could be attributed to the obvious decrease in the band gap, which could enhance the capacity of visible‐light absorption, and the presence of catalytic sites on the Chromium Schiff base complex was also a key factor for the photocatalytic performance, which could achieve high‐efficiency catalytic activity. Furthermore, these materials also exhibited a good recyclability with almost unchanged degradation efficiency after five recycling tests. Above these indicated that these materials mentioned had great potential in the field of wastewater treatment and antibiotic contaminant.