This study developed and characterized a γ-aminobutyric acid (GABA)-enriched yogurt fermented by Levilactobacillus brevis CGMCC1.5954. The GABA content in the yogurt was 147.36 mg/100 mL, which was 317.06% higher than that of the control group. Furthermore, there was a significant improvement in the aroma, hardness, adhesion, cohesiveness, and gelatinousness of yogurt. The chromatography and metabolomics analyses further confirmed the high GABA content in yogurt and its nutritional value, and the metabolic pathway for GABA production by L. brevis 54 was identified. A total of 58 volatile flavor compounds were identified using headspace solid-phase microextraction-gas chromatography-mass spectrometry, of which 2-nonanone and 2-heptanone may be responsible for the high odor score of GABA-enriched yogurt. This study developed a nutritious and unique GABA-enriched flavored yogurt, summarized the metabolic pathway of GABA, and provided a flavor fingerprint that could guide the production of specifically flavored yogurts.