The purpose of this study was to develop a method of combining molecular distillation and spray drying to concentrate and dry tea polyphenols extracts. Molecular distillation and spray drying of tea phenols extracts were performed using an orthogonal array design. The order of importance that influenced molecular distillation was distillation temperature > flux > rotational speed. The optimal conditions for concentration by molecular distillation were 70°C distillation temperature, 10 mL/min flux, and 1,200 n/min rotational speed. Inlet temperature was found to be the most important determinant of spray drying. The order of importance that influenced the spray drying was inlet temperature > feed flux > wind capacity > feed concentration. The optimal conditions for drying of tea polyphenols extracts by spray drying were determined as follows: 170°C distillation temperature, 3 mL/min feed flux, 30% feed concentration, and 30 m3/h wind capacity. Results of this study indicated that the combination of molecular distillation and spray drying was very suitable for the concentration and drying of tea polyphenols extracts. Using this approach to process tea polyphenol extracts can not only maintain the quality of tea polyphenols but also save time and energy.