Z-scheme mechanism was a promising approach to considerably enhance photocatalytic activity. In this work, the PDINH/NH2-UiO-66(Zr) (PNU) heterojunctions were made using a facile ball-milling method. As expect, the optimum PNU-1 composite acted as highly active photocatalyst with 97% Cr(VI) to be reduced within 60 min of LED light illumination. Moreover, the antibacterial rate almost reached 100% for E. coli and S. aureus in 4 h, which was more conspicuous than the others. The wider light absorption range, promoted charge separation because of Z-scheme mechanism and efficient generation of reactive 1O2, •O2-, and •OH contributed greatly to the enhanced photocatalytic activity. Meanwhile, the superior stability and repeatability of the composites were also demonstrated by five cyclic experiments and related physicochemical characterizations. Therefore, this work provides a novel insight for designing high-efficiency Z-scheme heterostructures between MOFs and organic PDINH for wastewater remediation.