Tea, leaf, or bud from the plant Camellia sinensis, make up some of the beverages popularly consumed in different parts of the world as green tea, oolong tea, or black tea. More particularly, as a nonfermented tea, green tea has gained more renown because of the significant health benefits assigned to its rich content in polyphenols. As a main constituent, green tea polyphenols were documented for their antioxidant, anti-inflammation, anticancer, anticardiovascular, antimicrobial, antihyperglycemic, and antiobesity properties. Recent reports demonstrate that green tea may exert a positive effect on the reduction of medical chronic conditions such as cardiovascular disease, cancer, Alzheimer’s disease, Parkinson’s disease, and diabetes. The health benefits of green teas, in particular EGCG, are widely investigated, and these effects are known to be primarily associated with the structure and compositions of its polyphenols. This Review focuses on the diverse constituents of green tea polyphenols and their molecular mechanisms from the perspective of their potential therapeutic function. Recent advances of green tea polyphenols on their bioavailability, bioaccessibility, and microbiota were also summarized in this article. Dietary supplementation with green tea represents an attractive alternative toward promoting human health.