The aroma of vanilla pods is mainly derived from vanillin. Microbial biotransformation reactions of vanillin precursors yield “natural” vanillin-related aroma metabolites. In this study, we coated vanilla pods with three edible microorganisms and observed the changes in tissues with a laser scanning microscope during early curing. In addition, the conducted volatile components analysis using gas chromatography-mass spectrometry (GC-MS) with ethanol extracts to investigate the differences in the aroma components of coated and uncoated microbial vanilla pods and to identify the correlation between processing and the oily luster of pods. The results demonstrate that the oily luster on the surface of vanilla pods coated with Bacillus subtilis subsp. subtilis is one of the necessary conditions for a high-quality vanilla product. Eight categories of compounds were found in the ethanol extract of vanilla pods. A total of 69 volatile components were analyzed. Different microbial species significantly influenced the volatile components, with 31 compounds not found in the control group. Furthermore, 30 odor and aroma compounds were identified. This study reveals the role of edible microbial coatings in enhancing the natural aroma of vanilla pods and offers possibilities for the development of new and unique vanilla aroma profiles.