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A novel and aqueous gel-casting process has been successfully developed to fabricate porous MgAl2O4 ceramics by using hydratable alumina and MgO powders as raw materials and deionized water as hydration agent. The effects of different amounts of deionized water on the hydration properties, apparent porosity, bulk density, microstructure, pore size distribution and compressive strength of the samples were investigated. The results indicated that the porosity and the microstructure of porous MgAl2O4 ceramics were governed by the amounts of deionized water added. The porous structure was formed by the liberation of physisorbed water and the decomposition of hydration products such as bayerite, brucite and boehmite. After determining the addition amounts of deionized water, the fabricated porous MgAl2O4 ceramics had a high apparent porosity (52.5–65.8%), a small average pore size structure (around 1–3 μm) and a relatively high compressive strength (12–28 MPa). The novel aqueous gel-casting process with easy access is expected to be a promising candidate for the preparation of Al2O3-based porous ceramics.