The high demand for nanomaterials in the field of industry and science has forced researchers to develop new synthesis methods that are more efficient, economical, and environmentally friendly. At present, the application of green synthesis has taken a great advantage over conventional synthesis methods because it helps with the control of the characteristics and properties of the resulting nanomaterials. In this research, ZnO nanoparticles (NPs) were synthesized by biosynthesis using dried boldo (Peumus boldus) leaves. The resulting biosynthesized NPs had a high purity, quasi-spherical shape with average sizes ranging from 15 to 30 nm and a band gap of ~2.8–3.1 eV. These NPs were used in the photocatalytic activity of three organic dyes. The results showed degradation of 100% methylene blue (MB) in 180 min, 92% methyl orange (MO) in 180 min, and 100% Rhodamine B (RhB) in 30 min of exposure. These results show that the Peumus boldus leaf extract is effective in the biosynthesis of ZnO NPs with good photocatalytic properties.