In this study, fullerene-modified lead molybdate (C60–PbMoO4) was prepared via a hydrothermal method, and characterized by X-ray diffraction, UV–vis diffuse reflection spectroscopy, high-resolution transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy. It was shown that the introduction of C60 reduces the crystallite size of PbMoO4, slightly influences the textual properties and optical characteristics (UV–vis absorption). The effect of C60 content on the photocatalytic activity of C60–PbMoO4 was studied in the photocatalytic degradation of rhodamine B under UV light and visible light irradiation. After modification with C60, the photocatalytic activity of PbMoO4 increased 3.8 times at a C60 weight ratio of 0.5 wt% under UV light irradiation, and 4.1 times at a C60 weight ratio of 5.0 wt% under visible light irradiation. The significant photocatalytic activity of C60–PbMoO4 was attributed to the excellent light absorption and charge separation on the interfaces between C60 and PbMoO4.