Remediation process produces high-value functional material from low-cost or valueless waste feedstock. Current research demonstrates an innovative solvothermal approach to effectively react sulfuric acid on polyethylene (PE) chains, modifying the PE at a moderate temperature. In this process, the polymer undergoes a cross-linking step above 120 °C, whereas above 500 °C, it transforms into turbostratic carbon structures. Scanning electron micrographs confirmed the free-standing carbon sheet architecture. Raman spectroscopy and X-ray diffraction verified the amorphous/disordered sp2/sp3 hybrid carbon structure in the produced carbons. A high Brunauer-Emmett-Teller surface area of 752.3 and 673.5 m2/g for low-density PE-derived carbon (LDPE-C) and high-density PE-derived carbon (HDPE-C), respectively, was recorded. Thermogravimetric analysis analysis established a total mass retention of 50 and 46% for LDPE and HDPE, respectively, from sulfonated materials. Li-ion battery composite anode comprising LDPE-C and HDPE-C, with a binder and a carbon additive (vs lithium), produced 230 and 350 mA h/g specific capacities for LDPE-C and HDPE-C, respectively, when cycled at room temperature at C/5 rate. Elevated temperature (50 °C) battery cycling produced 290 and 440 mA h/g specific capacities for LDPE-C and HDPE-C, respectively, at C/5 rate. On the basis of the literature survey, this is the first report, which demonstrates that a solvothermal sulfonation process followed by thermal treatment successfully converts waste LDPE and HDPE plastic bags to functional energy-storing carbons.