The invention provides a method for preparing aluminum oxide and other products from aluminiferous materials such as bauxite, high iron bauxite, alunite, kaoline, alumina, fly ash, coal gangue, aluminum ash, nepheline, clay and the like. The method comprises the following steps: (1) crushing, grinding and mixing the aluminiferous materials with ammonium sulfate and then roasting; (2) dissolving the roasted product (clinker aggregate) in water, and filtering to obtain aluminum ammonium sulfate solution and filter residues; (3) carrying out deferrization, aluminum deposition or recrystallization on the aluminium ammonum sulfate solution with ammonia to prepare aluminum oxide, and meanwhile, recycling the ammonium sulfate; (4) preparing silicon dioxide from the filter residues, and taking the remaining residues containing ferrum as the raw material for ironmaking. The method is suitable for treating various aluminiferous materials, has the advantages of simple technical process, simple equipment, no emission of solid, liquid and gas wastes, and no secondary pollution, and realizes the high-added-value green complex utilization of the aluminiferous materials such as bauxite, high ironbauxite, alunite, kaoline, alumina, fly ash, coal gangue, aluminum ash, nepheline, clay and the like.