Theanine, an amino acid unique to tea leaves, has been reported to exhibit stress-relieving effects. However, the stress-relieving effects of theanine (T) are greatly inhibited by caffeine (C) and epigallocatechin gallate (E), the main components of green tea, while being enhanced by arginine (A). Animal and clinical studies using matcha tea have shown that it can alleviate stress if the molar ratio of C and E against T and A (CE/TA) is less than 2. In general, the CE/TA ratio in tea leaves is reflected by the CE/TA ratio in the infused solution; however, it is not clear what infusion conditions would be expected to ensure a stress-relieving effect. In this study, to examine the stress-relieving effect of green-tea-infused solutions, the CE/TA ratio was measured under different infusion conditions. Furthermore, a study using a model solution consisting of C, E, T, and A revealed that a CE/TA ratio of at least less than 2 and a T content greater than 0.23 mM were required for stress reduction. Based on these results, we identified tea leaves and their infusion conditions that can be expected to reduce stress.