Instant teas are particularly rich in tea polyphenols and caffeine and have great potential as food ingredients or additives to improve the quality of food and enhance their nutritional and commercial value. To determine the relationships between raw material, drying method, and sensory and other quality attributes, instant teas were prepared from three tea varieties, namely black, green and jasmine tea, using two drying methods, namely spray-drying (SD) and freeze-drying (FD). Both the raw tea material and drying method influenced the quality of the finished instant teas. Black tea was quality stable under two drying, while green tea taste deteriorated much after SD. Jasmine tea must be produced from FD due to huge aroma deterioration after SD. FD produced instant tea with higher sensory quality, which was attributed to the lower processing temperature. Chemical compositional analysis and widely targeted metabolomics revealed that SD caused greater degradation of tea biochemical components. The flavonoids content changed markedly after drying, and metabolomics, combined with OPLS-DA, was able to differentiate the three varieties of tea. Instant tea preparations via SD often lost a large proportion of the original tea aroma compounds, but FD minimized the loss of floral and fruity aroma compounds. Changes in the tea flavonoids composition, especially during drying, contributed to the flavor development of instant tea. These results will provide an practicle method for high-quality instant tea production through choosing proper raw tea material and lowering down drying temperature with non-thermal technologies like FD.