Suan Rou (SR), a traditional fermented meat, is widely favored by consumers due to its unique flavor and characteristics. To study the relationship between the core differential micro-organisms and differential volatile organic compounds (VOCs) of SR from six regions of China, high-throughput sequencing (HTS) and gas-chromatography–ion mobility spectrometry (GC-IMS) technologies were used to analyze the correlation between micro-organisms and VOCs in SR from Xiangxi of Hunan, Rongshui of Guangxi, Zunyi of Guizhou, Jinping of Guizhou, Congjiang of Guizhou, and Libo of Guizhou. A total of 13 core micro-organisms were identified at the genus level. Moreover, 95 VOCs were identified in the SR samples by GC-IMS analysis, with alcohols, aldehydes, ketones, and esters comprising the major VOCs among all the samples. The results showed a strong correlation (|r| > 0.8, p < 0.05) between the core differential micro-organisms and differential VOCs, including four bacteria, five fungi, and 12 VOCs. Pediococcus, Debaryomyces, Zygosaccharomyces, and Candida significantly contributed to the unique VOCs of SR.