Till now, very few studies are focused on the interactive effect of wine-associated microbes including non-Saccharomyces, Saccharomyces, and lactic acid bacteria on modulating the organoleptic quality of black raspberry wines. In our study, Torulaspora delbrueckii, a widely studied non-Saccharomyces yeast, and Lactobacillus plantarum, a promising malolactic fermentation starter, were used in combination with S. cerevisiae for the production of black raspberry wine by three inoculation modes, i.e., sequential inoculation of three species (SE), co-culture of S. cerevisiae and L. plantarum (CO) and T. delbrueckii/S. cerevisiae sequential inoculation plus a spontaneous malolactic fermentation (SP), on the quality of black raspberry wine. A total of 34 aromatic compounds were identified by HS–GC–IMS technology. CO was found to boost the production of many fruity ester compounds, and scored the highest for ‘fruity’, ‘sweet’, and ‘total aroma’ attributes during sensory evaluation. SP was characterized by the lowest production of most volatile components and obtained the lowest rating. Principal component analysis showed that three samples were quite different from each other. Overall, CO had greater potential to be used in the production of black raspberry wine.