Epidemiological, clinical and experimental studies have established a positive correlation between green tea consumption and cardiovascular health. Catechins, the major polyphenolic compounds in green tea, exert vascular protective effects through multiple mechanisms, including antioxidative, anti-hypertensive, anti-inflammatory, anti-proliferative, anti-thrombogenic, and lipid lowering effects. (1) Tea catechins present antioxidant activity by scavenging free radicals, chelating redox active transition-metal ions, inhibiting redox active transcription factors, inhibiting pro-oxidant enzymes and inducing antioxidant enzymes. (2) Tea catechins inhibit the key enzymes involved in lipid biosynthesis and reduce intestinal lipid absorption, thereby improving blood lipid profile. (3) Catechins regulate vascular tone by activating endothelial nitric oxide. (4) Catechins prevent vascular inflammation that plays a critical role in the progression of atherosclerotic lesions. The anti-inflammatory activities of catechins may be due to their suppression of leukocyte adhesion to endothelium and subsequent transmigration through inhibition of transcriptional factor NF-kB-mediated production of cytokines and adhesion molecules both in endothelial cells and inflammatory cells. (5) Catechins inhibit proliferation of vascular smooth muscle cells by interfering with vascular cell growth factors involved in atherogenesis. (6) Catechins suppress platelet adhesion, thereby inhibiting thrombogenesis. Taken together, catechins may be novel plant-derived small molecules for the prevention and treatment of cardiovascular diseases. This review highlights current developments in green tea extracts and vascular health, focusing specifically on the role of tea catechins in the prevention of various vascular diseases and the underlying mechanisms for these actions. In addition, the possible structure-activity relationship of catechins is discussed.