To characterize the trace-element characteristics of chrysoberyl, we studied twenty-six chrysoberyl samples from various localities by using laser ablation inductively coupled plasma mass spectrometry (LA–ICP–MS), photoluminescence (PL), and ultraviolet–visible–near-infrared (UV–Vis–NIR) spectroscopy. Chemical analysis has confirmed the existence of trace elements, including Fe, Ti, Ga, Sn, B, Cr, and V. The phenomenon of ionic isomorphic substitution frequently occurs at lattice sites within chrysoberyl. Notably, the isomorphic substitution of Al3+ in octahedral sites is significant, with the primary substituting elements being Fe, Ti, Cr, V, Ga, and Sn. The PL spectra of chrysoberyl samples exhibit sharp peaks at 678 and 680 nm, which are attributed to Cr3+, even in samples in which the Cr concentration is below the detection limit of LA-ICP-MS. This demonstrates the high-sensitivity feature of PL spectroscopy. The UV–Vis–NIR spectra of chrysoberyl samples consistently exhibit a band at 440 nm, and strong double narrow bands near 367 nm and 375 nm are observed. These spectral features are associated with Fe3+ chromophores—specifically, Fe3+-Fe3+ pairs or clusters and Fe3+ ions, respectively. By combining LA–ICP–MS analysis and PL mapping on a sample exhibiting color zoning, it has been found that the darker sections contain a higher concentration of Cr compared to the lighter sections, while the concentrations of other elements remain largely consistent. In other words, subtle variations in Cr concentration may be the underlying cause of color zoning in chrysoberyl.