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Summary: Chestnut rice wine, also called banli mijiu (BLMJ), uses Chinese chestnut (Castanea mollissima Blume) in the fermentation of traditional glutinous rice wine. This study characterised the microbial communities and volatile compounds in BLMJ and explored their correlations. Headspace solid‐phase microextraction‐gas chromatography–mass spectrometry (HS‐SPME‐GC–MS) revealed that the major volatile compounds during BLMJ fermentation include eighteen important volatile compounds (OAV > 1). High‐throughput sequencing (HTS) demonstrated that the abundance and diversity of bacteria were significantly greater than those of fungi during the fermentation process. Among them, Kropensteria and Saccharomyces were the most abundant bacteria and fungi at the genus level during the fermentation of BLMJ. Spearman's correlation analysis revealed that eighteen important volatile compounds were significantly positively correlated with seven microbial genera (|r| > 0.9, P < 0.01), including six bacterial genera (Rhodococcus, Lactococcus, Pseudomonas, Janthinobacterium, Unclassified_f_Bacillaceae and Burkholderia‐Caballeronia‐Paraburkholderia) and one fungal genus (Saccharomyces). Therefore, these bacterias and fungi may be core functional microorganisms during BLMJ fermentation. The findings may provide important reference for mediating the microbial community during fermentation to improve the flavour of BLMJ. [ABSTRACT FROM AUTHOR]