Wastewater treatment has been bestowed with a plethora of materials; among them, metal-organic frameworks (MOFs) are one such kind with exceptional properties. Besides their application in gas adsorption and storage, they are applied in many fields. In orientation toward wastewater treatment, MOFs have been and are being successfully employed to capture a variety of aqueous pollutants, including both organic and inorganic ones. This review sheds light on the postsynthetic modifications (PSMs) performed over MOFs to adsorb and degrade recalcitrant. Modifications performed on the metal nodes and the linkers have been explained with reference to some widely used chemical modifications like alkylation, amination, thiol addition, tandem modifications, and coordinate modifications. The boost in pollutant removal efficacy, reaction rate, adsorption capacity, and selectivity for the modified MOFs is highlighted. The rationale and the robustness of micromotor MOFs, i.e., MOFs with motor activity, and their potential application in the capture of toxic pollutants are also presented for readers. This review also discusses the challenges and future recommendations to be considered in performing PSM over a MOF concerning wastewater treatment.