Strigolactones (SLs) are known to regulate plant architecture formation, nitrogen (N) and phosphorus (P) responses, and secondary metabolism, but their effects in tea plants remain unclear. We demonstrated that the application of a bioactive SL analogue GR24 either to tea roots or leaves initially stimulated but later inhibited catechins, theanine, and caffeine biosynthesis. GR24 treatment also promoted the accumulation of flavonols and insoluble proanthocyanidins in a time-and dose-dependent manner. GR24 influenced flavonoid and theanine biosynthesis genes, such as up-regulating CsTT2c, CsMYB12, and CsbZIP1, modulating N-responsive and assimilation genes (CsNRT1,1, CsGSI/TS1, CsHRS1, CsPHR1, CsNLA1, and CsLBD37/38/39), and repressing N/P transport and signaling genes (CsPHO2, CsPHT1s, CsNRT2,2, CsHHO1, and CsWRKY38). GR24-induced changes in secondary metabolites were also observed in the leaves of tea plants. GR24-regulated CsLBD37a interacted with CsTT8a and CsTT2c, repressing catechins biosynthesis by interrupting MBW complex formation. GR24 regulated caffeine biosynthesis and regulator genes CsS40 and CsNAC7 and may thereby suppress caffeine production. GR24 altered the transcriptomic profiles of multiple hormone biosynthesis and signaling genes that potentially regulate tea characteristic metabolism and N/P signaling. This study provides new insights into SL-induced transcriptional reprogramming that leads to changes in N/P nutrition, secondary metabolism, and hormone signaling in tea plants.