AbstractThe fast‐increasing interest in multivariate metal–organic frameworks (MTV‐MOFs) has burgeoned due to the possibility to create synergetic functions and achieve performance significantly better than their simple sum. In this work, the opportunities and the effects of multivariate functionalization of UiO‐66 on diverse properties important for photocatalytic water remediation: hydrolytic stability, bandgap energy, photoconduction, CrVI and CrIII adsorption capacity and kinetics, and CrVI to CrIII photoreduction efficiency, are explored. By developing a (Zr)UiO‐66‐NH2‐(OH)2‐NO2 multivariate material based on the combination of 2‐aminoterephthalate, 2,5‐dihydroxyterephthalate, and 2‐nitroterephthalate organic linkers in the same framework, a dual sorbent/photocatalyst is developed for water remediation with excellent properties: 1) enhanced adsorption efficiency of CrVI and CrIII ions, 2) improved photocatalytic conversion of CrVI to CrIII, and 3) with suitable chemical stability under acidic conditions for catalytic applications. This work represents a milestone for an emerging class of reticular materials that can synergistically use the properties of individual functionalities to solve complex problems beyond just the water remediation application discussed in this paper.