The tea plant is known as a fluorine accumulator. Fluoride (F) content in fresh leaves collected from 14 plantations in China was investigated. The F increased with maturity, and the F variation was remarkable in the tender shoots. Furthermore, significant negative relationships were observed between F content and the content of the quality parameters total polyphenols and amino acids. These substances are rich in young leaves and poor in mature ones. With regard to quality of tea products, the relationship with F content was studied using 12 brands of tea products in four categories: green tea, oolong tea, black tea, and jasmine tea collected from six provinces. The F level increased with the decline in quality and showed good correlation with the quality grades. The results suggest that the F content could be used as a quality indicator for tea evaluation.