This study was performed to compare nutritional compounds and physiological functions of five domestic and imported green tea cultivars at three time points. The five cultivars were compared for theanine, γ-aminobutyric acid, and catechin content by LC-MS/MS and HPLC. Furthermore, the five tea cultivars were functionally characterized with respect to antioxidant activity, brain cell protective effect, and inhibitions of α-glucosidase and HMG-CoA reductase activities. Among green tea cultivars, Chamnok had the highest content of catechins (198 mg/g DW), theanine (11.89 mg/g DW), and tannin (23.6 mg/g DW). Considering functional properties, Chamnok treatment resulted in the maximum viability of brain cells and reduced the cortisol content of SH-SY5Y cells. The inhibition of α-glucosidase and HMG-CoA reductase was the strongest following Chamnok treatment (72.9% and 69.8%, respectively). These results indicate that Chamnok could be optimal for consumption or favorable processing owing to its high nutritional compounds, such as theanine and catechin, and remarkable brain cell protective effects.