The demand for clean water free of pollution has become an urgent priority for humanity. Gd2Zr2O7 nanoparticles were successfully synthesized via sol–gel auto combustion as a type of pyrochlore to be used in the dye phytoremediation using a Fenton-like approach. Gd2Zr2O7 nanoparticles have been successfully prepared using a sol–gel auto-combustion strategy. The annealing process was performed in a furnace at 1100 °C for 2 h to form defect-fluorite structured Gd2Zr2O7 with space group Fm-3m. XRD analysis revealed that synthesized Gd2Zr2O7 nanoparticles were found to have crystallite sizes with lattice parameters of 28.5 nm and 10.524 + 0.02 Å, respectively. TEM micrographs showed the presence of a cubic-like structure with a size of about 17 nm. The band gap energy of the synthesized powders was found to be 3.8 eV relating to the impact of the crystallite size. The generated nanoparticles finally show a significant photo Fenton catalytic activity with an efficiency of 90% for the photocatalysis of crystal violet dye after 60 min. It was determined that the substantial absorption of Gd2Zr2O7 in the visible-light region, which was synergistically activated by both Gd3+ and Zr4+ ions, was the cause of the large surface area of the scattered microstructure and reactive OH. formation.