Scented tea is popular for its attractive flavor and health benefits, but cumbersome processing limits its production. In this study, freeze-dried optimized casein nano-embedded Citrus aurantium L. var. amara Engl. flower essential oil combined with phospholipids (CAVAO-CPNs) sustained-release aroma was used to efficiently process high-quality scented tea. Sensory evaluation and GC-E-Nose analysis indicated that new the newly processed scented tea (NST) had higher floral quality than the traditional scented tea (TST). SBSE-GC-MS identified 76 volatile compounds. Further analysis indicated that the levels of 21 key compounds increased significantly in scented tea, accounting for 94.4% and 69.3% of the total NST and TST, respectively. The total aroma content of NST was 9.08 times higher than that of TST. Relative odor activity values revealed six aroma characteristics dominated by floral aromas such as linalool, geranyl acetate etc. Correlation analysis indicated that NST has advantages over TST in terms of sensory intensity and the odor contribution of aroma compounds.