The alumina/polyimide multi-layers were fabricated by dry process using sputtering and vapor deposition polymerization. The alumina layer and polyamic acid layer as a polyimide precursor were coated on a Si substrate at room temperature. The layered structure was prepared under the continuous and discontinuous depositions; the former was to evaporate continuously under vacuum, while the latter was to expose in air after each layering process and to form the next layer under vacuum. After alternating depositions of up to 7 layers, the layered composites were heated to 573 K for 1 h to induce thermal imidization. Under the discontinuous deposition, cracks and delaminations occurred in the laminate. As for continuous deposition, the alumina/polyimide composite remained a multi-layered structure without cracks and delaminations.