The aroma-active compounds in the extra, first, and third grades of ylang-ylang essential oils (YYEO) from Comoros and Madagascar were identified by gas chromatography-mass spectrometry with olfactometry (GC-MS/O) using an aroma extract dilution analysis (AEDA) technique. In the previous study, the authors investigated differences in volatile compound profiles between YYEO of different grades and regions using GC coupled with a flame ionization detector (FID) and GC-MS. This study follows up with identification of the aroma-active compounds present in YYEO of various grades from both origins and to profile the aroma of those oils. For the first time, principal component analysis (PCA) on AEDA logarithmic flavor dilution (LFD) data was performed, in comparison with the corresponding PCA on GC-FID-MS data. Based on AEDA data, 21 aroma-active compounds were found across all samples and grades of YYEO, with 8 common ones previously identified by GC-FID. Linalool had the highest odor activity and is the major component of YYEO, followed by geraniol, although the latter only appeared as a much smaller peak in the chromatogram. Other trace compounds such as eugenol and vanillin were also found to be significant to the aroma of YYEO. Using PCA on resulting LFD data, YYEO from Comoros were found to have spicier odor qualities as compared to those from Madagascar. The main contributors that determine the difference in a spicy aroma profile of Comoros and Madagascar oils are vanillin, methyl eugenol, and trans-cinnamyl acetate.