Shaped porous ceramics have proven to be the most adapted materials for several industrial applications, both at low and high temperatures. Recent research has been focused on developing shaping techniques, allowing for a better control over the total porosity and the pores characteristics. In this study, macroporous alumina foams were fabricated by gel-casting using pre-expanded polymeric microspheres with average sizes of 40 μm, 20 μm, and 12 μm as sacrificial templates. The gel-casting method, as well as the drying, debinding, and presintering conditions were investigated and optimized to process mechanically strong and highly porous alumina scaffolds. Furthermore, a reliable model relating the amount of pre-expanded polymeric microspheres and the total porosity of the presintered foams was developed and validated by mercury intrusion porosimetry measurements. The electron microscopy investigation of the presintered foams revealed that the size distribution and the shape of the pores could be tailored by controlling the particle size distribution and the shape of the wet pre-expanded microspheres. Highly uniform and mechanically stable alumina foams with bimodal porosity ranging from 65.7 to 80.2 vol. % were processed, achieving compressive strengths from 3.3 MPa to 43.6 MPa. Given the relatively open pore structure, the pore size distribution, the presintered mechanical strength, and the high porosity achieved, the produced alumina foams could potentially be used as support structures for separation, catalytic, and filtration applications.