► The volatile compounds of cinnamon barks were studied by GC–MS and FTIR. ► GC–MS and FTIR, combined with chemometrics for the assessment of cinnamon quality. ► These methods are usable for determining species or their geographical distribution. ► Guangxi is a suitable cultivation site for C. loureirii and C. verum utilization. In this work, the volatile compounds of cinnamon barks from three species and seven habitats were detected and identified for the first time by GC–MS and FTIR analysis. GC–MS analysis indicated that the main compound in the volatile oils of nine samples was trans-cinnamaldehyde (66.28–81.97%). Cinnamomum loureirii had the highest volatile oil yield (3.08%) and in that yield was a high percentage of trans-cinnamaldehyde (81.97%). Cinnamomum verum contained significant quantities of eugenol, and Cinnamomum cassia had more abundant α-guaiene compared with C. loureirii and C. verum. Hierarchical cluster analysis, similarity evaluation and principal component analysis showed that the nine samples were effectively identified and evaluated. Load factor analysis revealed that the differences in the volatile compounds of the nine samples were mainly reflected in the aldehyde, alcohol, alkane and eugenol contents. Our research indicated that GC–MS and FTIR techniques, combined with chemometrics, proved to be an effective strategy for identifying the species and for determining their geographical distribution, especially in the assessment of cinnamon quality for use in raw herbal medicines.