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Upcycling is an attractive approach for valorization of waste plastics to valuable chemicals. Here we report the first case study of non-thermal plasma-assisted hydrogenolysis of high-density polyethylene (HDPE) to C1-C3 hydrocarbons. Light alkanes, predominately CH4, C2H6 and C3H8 with >95% selectivity, were obtained under ambient condition as result of favorable thermodynamics and fast reaction kinetics. The findings demonstrated that hydrogenolysis that typically demands above 300 °C with thermal catalysis can occur at room temperature in assistance of non-thermal plasma. This proof-of-concept study showcases a novel strategy for upcycling of plastics to valuable hydrocarbons under ambient condition.