This work aimed to investigate the effect of salt concentration on the quality and microbial community of pickled peppers during fermentation, and the cross-correlation between microorganisms and quality was also revealed. The results showed that 9 volatile flavor compounds were unique to the low salt concentration group (D group), which also contained higher content of FAA, lactic acid and acetic acid than high salt concentration group (G group). Meanwhile, the samples of D2 group have a better texture properties. Firmicutes, Proteobacteria, Ascomycota, Lactobacillus, Pectobacterium, and Pseudomonas were detected as the main microbial community during the fermentation with different salt concentrations. Furthermore, the correlations analysis results indicated that the salt concentration has a significant effect on the microbial community of pickled peppers (p < 0.001), and Pediococcus, Lactobacillus, Cedecca, Issatchenkia, Pichia, Kazachstania, and Hanseniaspora were significantly correlated with flavors, which played crucial roles in the unique flavor formation of pickled peppers.