It is interesting to obtain catalysts to degrade organic dye pollutants at room temperature for simultaneous purposes of environment-treating and energy-saving. In this work, a novel ZrHIO6⋅46⋅4H2O catalyst was synthesized by reacting ZrO(NO3)23)2 with H5IO6 in aqueous nitric acid. The catalyst was found effective in degradation of rhodamine B (RhB) or methylene blue (MB) dyes at room temperature without light illumination. We used the ultraviolet–visible (UV–Vis) absorption spectra of dye solution as well as X-ray photoelectron spectroscopy (XPS) of ZrHIO6⋅46⋅4H2O to confirm that the dye degradation was due to its catalytic role. Importantly, the ZrHIO6⋅46⋅4H2O catalyst can be recycled five times without obvious activity loss and it achieved higher mineralization efficiency than the previously reported analogue in the degradation experiments.