In this study, seventeen faceted gem-quality chrysoberyls exhibiting an attractive canary yellow color were investigated using a variety of gemological, spectral, and chemical methods. Microscopic observation revealed the presence of distinct growth lines and inclusions, including CO2 fluids, carbon, and crystals of mineral such as calcite, quartz, sillimanite, and mica, identified by the Raman spectrum. The FTIR spectra showed the characteristic peaks of 2405 and 2160 cm−1 and a 3223 cm−1 peak in all samples, which can be accompanied by the 3112 cm−1 shoulder, 3301, and 3412 and 3432 cm−1 peaks. The UV-Vis spectra showed an Fe-related peak at 440 nm, along with the 650–660 nm band and the absorption band in the blue zone of visible light. Chemical analyses via EDXRF showed a composition poor in V and Cr and rich in Fe. The spectral and chemical results could help explain the origin of the canary yellow color, which originates from the abundant amount of Fe with very little influence from Cr and V.