Ceramic-based hollow spheres are considered a great driving force for many applications such as offshore buoyancy modules due to their large diameter to wall thickness ratio and uniform wall thickness geometric features. We have developed such thin-walled hollow spheres made of alumina using slip casting and sintering processes. A diameter as large as 50 mm with a wall thickness of 0.5–1.0 mm has been successfully achieved in these spheres. Their material and structural properties were examined by a series of characterization tools. Particularly, the feasibility of these spheres was investigated with respect to its application for deep sea (>3000 m) buoyancy modules. These spheres, sintered at 1600 °C and with 1.0 mm of wall thickness, have achieved buoyancy of more than 54%. As the sphere’s wall thickness was reduced (e.g., 0.5 mm), their buoyancy reached 72%. The mechanical performance of such spheres has shown a hydrostatic failure pressure above 150 MPa, corresponding to a rating depth below sea level of 5000 m considering a safety factor of 3. The developed alumina-based ceramic spheres are feasible for low cost and scaled-up production and show great potential at depths greater than those achievable by the current deep-sea buoyancy module technologies.