Soil acidification in tea plantations leads to an excessive heavy metal content in tea, decreasing its yield and quality. How to apply shellfish and organic fertilizers to improve soil and ensure the safe production of tea is still not clear. A two-year field experiment was conducted in tea plantations in which the soil was characterized by a pH of 4.16 and concentrations of lead (Pb) (85.28 mg/kg) and cadmium (Cd) (0.43 mg/kg) exceeding the standard. We used shellfish amendments (750, 1500, 2250 kg/ha) and organic fertilizers (3750, 7500 kg/ha) to amend the soils. The experimental results showed that compared with the treatment without any amendment (CK), the soil pH increased by 0.46 on average; the soil available nitrogen, phosphorus, and potassium contents increased by 21.68%, 19.01%, and 17.51% respectively; and the soil available Pb, Cd, Cr, and As contents decreased by 24.64%, 24.36%, 20.83%, and 26.39%, respectively. In comparison to CK, the average yield of tea also increased by 90.94 kg/ha; tea polyphenols, free amino acids, caffeine, and water extract increased by 9.17%, 15.71%, 7.54%, and 5.27%, respectively; and the contents of Pb, Cd, As, and Cr in the tea decreased significantly (p < 0.05) by 29.44-61.38%, 21.43-61.38%, 10.43-25.22%, and 10.00-33.33%, respectively. The greatest effects on all parameters occurred with the largest amendment of both shellfish (2250 kg/ha) and organic fertilizer (7500 kg/ha) combined. This finding suggests that the optimized amendment of shellfish could be used as a technical measure to improve the health quality of both soil and tea in acidified tea plantations in the future.