A combined bottom-up and top-down route was developed for the template-free synthesis of mesoporous CeO 2 powders using Ce(NO 3 ) 3 $6H 2 O, NH 4 HCO 3 , H 2 O 2 , and H 2 O as starting reagents. The flake-like Ce 2 (CO 3 ) 3 $8H 2 O precursor was etched by H 2 O 2 , and CeO 2 nucleated in situ with built-in equiaxed particles. Pores formed on the flakes owing to the loss of by-products of H 2 O and CO 2 . The formation of the mesostructured CeO 2 could also be explained by the large change in volume induced as a result of the difference in density between Ce 2 (CO 3 ) 3 $8H 2 O and CeO 2 . Accordingly, the original flake-like morphology of Ce 2 (CO 3 ) 3 $8H 2 O was not preserved upon pore formation and during continuous stirring in the synthesis. A subsequent hydrothermal treatment destroyed the loose aggregates of CeO 2 derived from the reaction between H 2 O 2 and Ce 2 (CO 3 ) 3 $8H 2 O. Rearrangement of the CeO 2 particles via a dissolution-recrystallization process occurred under certain temperatures and pressures. Consequently, CeO 2 particles with coarser sizes, smoother surfaces, and mesoporous structures were obtained. The specific surface area of the particles was 166.5 m 2 g À1 after hydrothermal treatment at 200 C for 24 h. The mesoporous CeO 2 particles possessed better adsorption capacities of acid orange 7 dye than basic orange 2 dye in the absence of pH pre-adjustments. The saturated adsorption amount of acid orange 7 dye was 510.2 mg g À1 at 298 K based on Langmuir linear fitting of the experimental data.