The newest method for recycling waste linear low-density polyethylene (LLDPE) is the thermo-catalytic degradation technique known as catalytic pyrolysis. Typically, it is limited by 500–800 °C high temperatures. Catalytic pyrolysis releases toxins and forms harmful carbonized char. The current study is based on exposing wasted LLDPE to different gamma irradiation doses and then pyrolysis in castor oil (150–300 °C). The output product of Ir-(rLLDPE) is turned into another compound with a new structural architecture (sponge-like). SEM analysis confirms conversion, showing sponge-like spicules and layers. Ir-(rLLDPE) is sponge-like with a soft, malleable, absorbent texture. The DSC demonstrates altered thermal properties, with a melting point at 121 °C splitting into two peaks (endothermic at 117 °C and exothermic at 160 °C). The exothermic peaks signify the curing process of the sponge-like material. Ir-(rLLDPE) is assessed as an adsorbent for aqueous oils and solvents. The study examines irradiation doses, pyrolysis temperature, and time on adsorbent capacity. The oil removal obeys the Langmuir isotherm with monolayer adsorption, with a maximum adsorption capacity of 24.75 g/g of waste oil and 43 g/g of 1,1,2,2-tetrachloroethane. Squashing maintains adsorption after 20 reuses. Data shows sponges effectively clean marine oil spills and solvents.