A simple synthesis for highly ordered mesoporous Ce1-xZrxO2 solid solutions with various Ce/Zr ratios is achieved. Structural characterization with small-angle and wide-angle PXRD, vis-Raman spectra, and TEM methods reveals that the Ce1-xZrxO2 have a 2D hexagonal mesostructure with crystalline walls. The Pt-loaded meso-Ce0.5Zr0.5O2 catalyst is tested for CO oxidation and cyclohexene hydrogenation and exhibits high catalytic activity, demonstrating that the as-prepared mesoporous Ce1-xZrxO2 have potential catalytic applications.