The management of plastic waste is a massive challenge and the recycling of plastics for newer applications is a potential solution. This study investigates the feasibility of using polyethylene terephthalate (PET) powder in cementitious composites. The changes in the strength and microstructure of Portland cement incorporating PET powder with different replacement ratios were systematically analyzed through the measurements of compressive strength, isothermal calorimetry, X-ray diffraction, thermogravimetric analysis, and Raman spectroscopy. In addition, the possible chemical changes of cement paste samples were studied upon exposure to different conditions, including deionized water, seawater, and simulated pore solution. Based on the test results and analysis, no apparent chemical changes were observed in the cement paste samples, regardless of the exposure conditions. In contrast, the PET powder incorporated into concrete exhibited remarkable changes, which may have occurred during the mixing process. The results also suggested that the maximum replacement ratio of PET powder should be less than 10% of the binder (by mass) to minimize its influence on cement hydration, due to the interaction between water and PET. The PET-containing samples showed the presence of calcium aluminate hydrates which were absent in the neat paste sample.