Currently, several organic dyes found in wastewater cause severe contamination problems for flora, fauna, and people in direct contact with them. This research proposes an alternative for the degradation of polluting dyes using ZnO nanoparticles (NPs) synthesized by an ecological route using leaf and root extracts of Ambrosia ambrosioides as a reducing agent (with a weight/volume ratio = 4%). Scanning Electron Microscopy (SEM) was used to determine the morphology, showing an agglomeration of cluster-shaped NPs. Using Transmission Electron Microscopy (TEM), different sizes of NPs ranging from 5 to 56 nm were observed for both synthesized NPs. The composition and structure of the nanomaterial were analyzed by infrared spectroscopy (FT-IR) and X-ray diffraction (XRD), showing as a result that the NPs have a wurtzite-like crystalline structure with crystallite sizes around 32–37 nm for both samples. Additionally, the bandgap of the NPs was calculated using Ultraviolet Visible Spectroscopy (UV–Vis), determining values of 2.82 and 2.70 eV for the NPs synthesized with leaf and root, respectively. Finally, thermogravimetric analysis demonstrated that the nanoparticles contained an organic part after the green synthesis process, with high thermal stability for both samples. Photocatalytic analysis showed that these nanomaterials can degrade four dyes under UV irradiation, reaching 90% degradation for methylene blue (MB), methyl orange (MO) and Congo red (CR) at 60, 100 and 60 min, respectively, while for methyl red (MR) almost 90% degradation was achieved at 140 min of UV irradiation. These results demonstrate that it is effective to use Ambrosia ambrosioides root and leaf extracts as a reducing agent for the formation of ZnO NPs, also evidencing their favorable application in the photocatalytic degradation of these four organic dyes.