Thanks to a bottom-up design of metals and organic ligands, the library of metal-organic frameworks (MOFs) has seen a conspicuous growth. Post-synthetically modified MOFs comprise a relatively smaller subset of this library. Whereas the approach of post-synthetic modification was seminally introduced for MOFs in the early 1990s, the earliest examples of post-synthetically modified MOFs are only congruous with adsorption and catalysis. The utility of PSM-derived MOFs for the sensing and capture of water contaminants is relatively niche. Arguably though, an increasing number of post-synthetically modified MOFs are finding relevance in the context of water pollutant remediation. In this article, we review the recent advances in this area and propose a structure-function relationship-guided blueprint for the future outlook.