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The effects of foliar phenylalanine application during veraison (FPV) on phenolic biosynthesis and correlation between phenolic compositions and antioxidant activities in Cabernet Sauvignon grown in field and greenhouse were investigated. Solutions with 69 and 138 mg N/vine phenylalanine (Pe1 and Pe2, respectively) and an aqueous solution without nitrogen (CK) were sprayed three times during veraison. FPV significantly improved antioxidant activities in grapes using the two culture methods. The most contributory phenolic compositions to antioxidant activities were anthocyanins and stilbenes following FPV compared with CK. Phenylalanine metabolism, abscisic acid content, and expression levels of VvPAL, VvCHS, VvF3H, VvUFGT, and VvSTS in the phenolic synthesis pathway were increased from the first FPV to harvest. Although Pe2 significantly increased total phenolic contents than Pe1, antioxidant parameters were not markedly affected by the phenylalanine dose. Our finding revealed that FPV was a useful fertilization method to enhance antioxidant activities in grapes in nitrogen-deficient vineyards.