Sustainable pollutants remedial is focussed by using surfactant-free ZnS nanoparticles (NPs) which are decorated with elemental-type sulfur defects (Es). Such functional ZnS NPs enable complete and rapid degradations of dye, drug (paracetamol, tetracycline), and explosive (trinitro-phenol) with UV to visible light irradiations. The evidences of Es formation are established by XPS, PL, and chemical reaction studies. HRTEM, XRD, EELS, UV–vis. absorption, PL, and Raman measurements have provided structural details of nanoparticles as well as confirmation on the critical role of Es towards the harvest of visible light. The highest carrier lifetime (5.8 µSec) of Es with a huge photocurrent (1.4 µA/cm2) has revealed further insights of the exceptional degradation abilities of ZnS nanocatalysts of pollutants. The nanocatalyst decays pollutants completely under direct sunlight and shows ∼24 and ∼2.5 times better performances than the commercial ZnS and TiO2 (P25), respectively. Thus, impeccable photocatalysis efficacy of defects decorated ZnS nanocatalysts under a wide range of wavelengths of light is demonstrated. The study opens up further energy harvesting applications.