A sol-gel granulation process was developed to prepare porous nanostructured γ-alumina granules as supports for catalysts and adsorbents. The process, which starts with an aqueous sol of gelatinous boehmite, involves droplet formation, gelation in paraffin oil, conditioning in ammonia solution, and drying and calcination in air under controlled conditions. The γ-Al2O3 granules prepared are 1–3 mm-dia. spherical particles with large surface area (380 m2/g) and pore volume (0.5 cm3/g), uniform pore-size distribution (20–60 Å), and controllable average pore size (35 Å). These sol-gelderived granules have excellent mechanical properties with crush strength (>100 N per granule) and attrition resistance (<0.01 wt. %/h), much better than the commercial alumina and zeolite granules. Supported CuO sorbents were prepared on these granules for SO2 removal applications. The alumina-supported CuO sorbents contain higher loading of well-dispersed CuO and better sulfation properties than similar sorbents reported in the literature.