Nowadays, the use of natural materials and especially “waste” valorization has evolved and attracted the wide attention of scientists and academia. In this regard, the use of rice husk (RH) powder as a naturally abundant and cheap byproduct material is gaining superior attention. However, improving the physicochemical properties of such RH is still under research. In the current investigation, the modification of rice husk (RH) via γ-irradiation has shown to be a promising green tool to meet such a need. Clean, prepared, powdered RH samples were subjected to various γ-radiation doses, namely 5, 10, 15 and 25 kGy, and the corresponding samples were named as RH-0, RH-5, RH-10, RH-15, RH-15 and RH-25. Then, the samples were characterized via scanning electron microscopy (SEM). After irradiation, the samples showed an increase in their surface roughness upon increasing the γ-radiation up to 15 kGy. Furthermore, the sorption capacity of the irradiated RH samples was investigated for eliminating Urolene Blue (UB) dye as a model pharmaceutical effluent stream. The highest dye uptake was recorded as 14.7 mg/g, which corresponded to the RH-15. The adsorption operating parameters were also investigated for all of the studied systems and all adsorbents showed the same trend, of a superior adsorption capacity at pH 6.6 and high temperatures. Langmuir and Freundlich isotherm models were also applied for UB adsorption and an adequate fitted isotherm model was linked with Langmuir fitting. Moreover, the pseudo-second-order kinetic model provided the best fit for the adsorption data. Experimental assays confirmed that the UB dye could be successfully eradicated feasibly from the aqueous stream via a sustainable green methodology.