With the widespread use and increasing consumption of PET, the amount of waste PET is growing rapidly, and the accompanied environmental problems will become more and more serious. Therefore, the recycling and reuse of PET are of great significance for not only saving resources but also solving environmental issues. In this study, Methylcellulose (MC) composites reinforced with waste plastics polyethylene terephthalate (PET) were prepared by casting an MC/PET solution with a varying mass ratio of MC to PET. Systematic investigations were performed to reveal the effect of the MC/PET mass ratio on the mechanical property, chemical structure, and thermal properties. The resultant findings indicate that the addition of 3% waste plastics PET to MC could notably enhance the tensile strength by about 24% as compared with neat MC. Interestingly, the elongation of the MC/PET composite kept increasing with increasing waste plastics PET. At the same time, thermal compression treatment could also enhance the mechanical properties of the composite. Moreover, the composites also displayed higher thermal stability than MC. In addition, the crystallinity and morphology of the composite were estimated by XRD and SEM.