The contamination of environmental waters with heavy metals and radionuclides is increasing because of rapid industrial and population growth. The removal of these contaminants from water via adsorption onto metal nanoparticles is an efficient and promising technique to abate the toxic effects associated with these pollutants. Among metal nanoparticle adsorbents, zinc oxide nanoparticles (ZnONPs) have received tremendous attention owing to their biocompatibility, affordability, long-term stability, surface characteristics, nontoxicity, and powerful antibacterial activity against microbes found in water. In this review, we considered the adsorption of heavy metals and radionuclides onto ZnONPs. We examined the isotherm, kinetic, and thermodynamic modeling of the process as well as the adsorption mechanism to provide significant insights into the interactions between the pollutants and the nanoparticles. The ZnONPs with surface areas (3.93 to 58.0 m2/g) synthesized by different methods exhibited different adsorption capacities (0.30 to 1500 mg/g) for the pollutants. The Langmuir and Freundlich isotherms were most suitable for the adsorption process. The Langmuir separation factor indicated favorable adsorption of all the pollutants on ZnONPs. The pseudo-second-order kinetics presented the best for the adsorption of the adsorbates with regression values in the range of 0.986–1.000. Spontaneous adsorption was obtained in most of the studies involving endothermic and exothermic processes. The complexation, precipitation, ion exchange, and electrostatic interactions are the probable mechanisms in the adsorption onto ZnONPs with a predominance of complexation. The desorption process, reusability of ZnONPs as well as direction for future investigations were also presented.