ABSTRACT A large number of toxic, flammable, and volatile organic solvents are used in the organic tape‐casting process, which have significant adverse effects on both the natural environment and human health. This study reports an aqueous polymer–ceramic slurry suitable for tape casting using water as the solvent instead of traditional organic solvents. The effects of chemical additives (dispersant, binder, plasticizer, and defoamer) on the viscosity, stability, and bubble content of the water‐based alumina ceramic slurry used for aqueous tape casting were investigated. The results showed that when the dispersant (ammonium polyacrylate) (PAA‐NH 4 ) and defoaming agent (M15‐01) contents were 1.5 and 0.1 wt%, respectively, and the ratio of binder (polyvinyl alcohol) (PVA) to plasticizer (glycerol) was 0.6, the surface of the green tape obtained by aqueous tape casting was the smoothest and flattest. Moreover, the alumina ceramic substrate of a size of 100 mm × 100 mm obtained by cutting and sintering the green tape exhibited dielectric constant, thermal conductivity, and breaking tenacity of 9.73, 23.16 W m −1 K −1 , and 4.34 MPa m 1/2 , respectively, making it an ideal candidate for high‐power integrated circuits. This study not only addresses the environmental and health concerns associated with organic solvents but also presents a promising solution for developing advanced aqueous polymer–ceramic slurries.