To protect skin from harmful ultraviolet (UV) radiation, there has been a resurgence in the use of natural dyes with metal mordants to reduce contamination by advanced chemicals. This study achieved natural dyeing in violet and yellow colors from Gromwell red roots and Cape jasmine seeds for UV-protective materials. The dyed fabrics were subjected to zinc oxide (ZnO) and polyphenol treatments, as well as copper post-mordanting. The SEM, TEM, and XRD tests showed that the ZnO nanoparticles, with hexagonal crystal structures, stuck to the fiber surfaces, and twisted strands resulted in the K/S reduction. First, this study found that the untreated cotton in violet, despite the highest K/S, faded the most intensely when exposed to UV. The color variation of untreated polyester was narrow, with little change in L, a*, and K/S. The color change of yellow-dyed samples treated with ZnO/polyphenol was not considerable in yellowness (b*: 28.838), while the violet fabrics displayed a significant decrease in K/S and an increase in b*. The combination of ZnO and polyphenol treatment improved UV absorption at 350 to 250 nm. Among the Cu-mordanted fabrics after ZnO/phenols treatment, the violet cotton turned reddish from blueish (negative to positive b*), with a hue change of 316° to 59° and the highest ΔE (25.90 ± 4.34) after UV exposure. In this study, the combination of ZnO/polyphenol with Cu-mordants allowed the Cape jasmine-dyed polyester to achieve a minimum ΔE as well as to keep its chroma and hue after UV exposure.