Tan is a local fat-tail sheep that is famous for its great eating quality but with little attention to its meat metabolome. The aim of this study was to investigate Tan-lamb meat metabolome as well as the key rumen bacteria related to the beneficial compound deposition in the muscle using untargeted and targeted metabolomics under different feeding regimes: indoor feeding (F), artificial pasture grazing with indoor feeding (GF), and pure artificial pasture grazing (G). The untargeted metabolome was detected by ultraperformance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry. Ruminal bacterial communities were detected by 16S rRNA sequencing. Using untargeted metabolomics, the main three altered metabolic pathways in the lamb, including amino acid, lipid, and nucleotide metabolisms, were found in the G group compared to the GF and F groups. Increased N-acetyl-L-aspartic acid, N-acetylaspartylglutamate, acetylcarnitine, and L-carnitine, but decreased carnosine and creatinine, were the main newly found G group-associated metabolites, which might contribute to the improved lamb meat functional quality. Compared to the F group, the G group feeding increased the contents of sweet amino acids (e.g., glycine, alanine, serine, and threonine) and umami amino acids (e.g., glutamic acid and aspartic acid) in the muscle, and G and GF groups increased the level of meat polyunsaturated fatty acid (PUFA), especially the concentration of n3 PUFA, and reduced n6/n3 in the muscle by targeted metabolomics. The abundance of ruminal Moryella was decreased, and Schwartzia and Anaeroplasma were increased in the G group, which were both strongly correlated with the n3 PUFA and other functional compounds in the muscle of lambs. In conclusion, artificial pasture grazing modified the meat amino acid and fatty acid composition as well as the related biological pathways through rescheduling the rumen bacterial community, which would be a better selection for production of healthier lamb meat products.