In this study, a unique tea cultivar ‘Anxi kucha’ was discovered for the first time, which is rich in both secondary metabolites. In the targeted data, theacrine (17.44 mg/g) was detected only in the ‘Anxi kucha’ tea plant in the test materials. The content of EGCG3"Me in ‘Anxi kucha’ (11.25mg/g), ‘Tieguanyin’ (5.32mg/g) and ‘Fudingdabaicha’ (0.93mg/g) showed high, medium and low changes. Through proteomics and transcriptomics, it was identified that the key pathways for the synthesis of theacrine and EGCG3"Me were the purine metabolism pathway and the flavonoid biosynthesis pathway, respectively. Combined proteome-transcriptome-metabolome analysis showed that SAMS3, APRT1, IMPDH, and TCS1 were the main enzymes promoting theacrine synthesis; CHI1, CHI2, FLS2 and LAR1 were the main enzymes that promote the synthesis of EGCG3"Me. The results of transcription factor analysis showed that MYB4 and bHLH74 had positive regulatory effects on the synthesis of theacrine and EGCG3"Me. Theacrine and EGCG3"Me are both bitter compounds. This study provides a valuable material rich in theacrine and EGCG3"Me, which provides a material basis for further development and utilization in the field of tea health food and a theoretical basis for studying the functional components of tea.