The valorization technique successfully transformed waste polyethylene terephthalate (PET) into valuable carbon nanomaterial (CN)/graphene, while doped and undoped ZnO nanopowders were synthesized via sol–gel methods. Utilizing XRD, BET, TEM, EDX, FTIR, and TGA analyses, the synthesis of sp2 2D sheet, pristine, and doped ZnO nanostructures was confirmed. Solid-state gas sensor devices, tested under 51% relative humidity (RH), 30 °C ambient temperature, and 0.2 flow rate, exhibited a 3.4% enhanced response to H2 gas compared to CO2 at 50 ppm concentrations over time. Notably, the ZnO/CN sensor surpassed CN and ZnO alone, attributed to CN dopant integration with decreasing order of response performance as ZnO/CN > CN > ZnO. This study underscores the efficacy of valorization techniques in generating high-value carbon nanomaterials and their efficacy in bolstering gas sensor performance, with ZnO/CN demonstrating superior response capabilities.