Tea has received attention due to its phytochemicals. For the direct use of tea germplasm in breeding programs, a core collection that retains the genetic diversity and various phytochemicals in tea is needed. In this study, we evaluated the content of eight phytochemicals over two years and the genetic diversity through 33 SSR (simple sequence repeats) markers for 462 tea accessions (entire collection, ENC) and developed a target-oriented core collection (TOCC). Significant phytochemical variation was observed in the ENC between genotypes and years. The genetic diversity of ENC showed high levels of molecular variability. These results were incorporated into developing TOCCs. The TOCC showed a representation of the ENC, where the mean difference percentage, the variance difference percentage, the variable rate of coefficient of variance percentage, and the coincidence rate of range percentage were 7.88, 39.33, 120.79, and 97.43, respectively. The Shannon’s diversity index (I) and Nei’s gene diversity (H) of TOCC were higher than those of ENC. Furthermore, the accessions in TOCC were shown to be selected proportionally, thus accurately reflecting the distribution of the overall accessions for each phytochemical. This is the first report describing the development of a TOCC retaining the diversity of phytochemicals in tea germplasm. This TOCC will facilitate the identification of the genetic determinants of trait variability and the effective utilization of phytochemical diversity in crop improvement programs.