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The Penglai sapphires are mainly hosted in alkaline basalts and derived in alluvial sediments. Previous studies have investigated the formation of the Penglai sapphires; however, the genesis of color zoning remains ambiguous. In this paper, we report spectral and chemical composition data of sapphires using ultraviolet–visible spectroscopy (UV–Vis), Fourier transform infrared spectroscopy (FTIR), and laser-ablation–inductively coupled plasma–mass spectrometry (LA–ICP–MS). The results show that the Penglai sapphire has a magmatic origin, mostly showing various shapes of incomplete girdles, barrels, and flakes. The content of Ti in rims is higher than in cores of color-banded sapphire, which results from ubiquitous Ti-bearing inclusions within grown bands. The main chromophore of the deep-blue core is Fe²⁺-Ti⁴⁺, which pairs with Fe³⁺-Fe³⁺, Cr^3+, and V³⁺ in the core, likely producing purple-hued blue in an oxidizing environment. The yellowish-brown rim is due to Fe³⁺ and Cr³⁺ in a reduced environment. Compared with the basaltic sapphires worldwide, the Fe content is moderately higher than those of most Asian sapphires but obviously lower than those of Changle sapphires in Shandong, China, and overlaps with those of African sapphires.