To elucidate the molecular mechanisms underlying the differential metabolism of albino (white), green, and purple pericarp coloration, biochemical profiling and transcriptome sequencing analyses were performed on three different tea pericarps, Zhongbaiyihao (Camellia sinensis L. var. Zhongbai), Jinxuan (Camellia sinensis L. var. Jinxuan), and Baitangziya (Camellia sinensis L. var. Baitang). Results of biochemical analysis revealed that low chlorophyll content and low chlorophyll/carotene ratio may be the biochemical basis for albino characteristics in the ‘Zhongbaiyihao’ pericarp. The differentially expressed genes (DEGs) involved in anthocyanin biosynthesis, including DFR, F3′5′H, CCoAOMT, and 4-coumaroyl-CoA, were highly expressed in the purple ‘Baitangziya’ pericarp. In the chlorophyll synthesis of white pericarp, GUN5 (Genome Uncoupled 5) and 8-vinyl-reductase both showed high expression levels compared to the green one, which indicated that albino ‘Zhongbaiyihao’ pericarp had a higher chlorophyll synthesis capacity than ‘Jinxuan’. Meanwhile, chlorophyllase (CLH, CSS0004684) was lower in ‘Baitang’ than in ‘Jinxuan’ and ‘Zhongbaiyihao’ pericarp. Among the differentially expressed transcription factors, MYB59, WRKY41-like2 (CS ng17509), bHLH62 like1 (CS ng6804), and bHLH62-like3 (CSS0039948) were downregulated in Jinxuan pericarp, suggesting that transcription factors played a role in regulating tea pericarp coloration. These findings provide a better understanding of the molecular mechanisms and theoretical basis for utilizing functional components of tea pericarp.