A limestone relief fragment with a figure in a winged disk from the fifth-century BCE Hall of 100 Columns at Persepolis in southwestern Iran that entered the Harvard Art Museums’ collections in 1943 preserves significant traces of its original coloration and has played a key role in the rediscovery of polychromy at the Achaemenid Persian capital. After tracing the fragment’s journey to Cambridge, MA, this article presents the results of recent technical studies of its pigment remains, including visible light-induced infrared luminescence (VIL) imaging, X-ray fluorescence (XRF) spectroscopy, and the analysis of micro samples by Raman spectroscopy, Fourier transform infrared (FT-IR) spectroscopy, scanning electron microscopy (SEM), and polarizing light microscopy (PLM). The new scientific data is compared to the findings of ongoing investigations of polychromies at Persepolis and other Achaemenid Persian sites and evaluated for the information it can and cannot provide on the original appearance of the figure in the winged disk, likely the Zoroastrian god Ahuramazda. The article reviews past attempts at reconstructing the relief’s coloration and the assumptions that guided them, recounts the experience of creating a tangible three-dimensional color reconstruction for an exhibition, and concludes with some general thoughts on the valuation of colorfulness.