Large-leaf yellow tea (LYT) is a yellow tea product with a specific aroma characteristic and is enjoyed with increasing enthusiasm in China. However, its key odorants are still unknown. In this study, 46 odorants in the headspace and vacuum-distillate of the tea infusion were identified via aroma extract dilution analysis. Sixteen compounds were newly found in LYT infusion. They were present in the highest flavor dilution factors together with 2-ethyl-3,5-dimethylpyrazine. All odorants were quantitated to evaluate their own odor activity values (OAVs). High OAVs were found for 2-methylbutanal (malty, 210), (E,E)-2,4-heptandienal (fatty/flowery, 170), 2-methylpropanal (malty, 120) and 2,3-diethyl-5-methylpyrazine (earthy/roasty, 110). An aroma recombinate consisting of 17 odorants (all OAVs ≥ 1) in an odorless nonvolatile LYT matrix mimicked the overall aroma of the original infusion, verifying the successful characterization of key aroma components in a LYT beverage. The knowledge of key odorants obtained showed potential for simplifying industrial flavor optimization of the LYT product.