The invention provides a method for removing iron and alunite in a halloysite ore and belongs to the field of deep processing of ores. The method comprises the four steps: (1) preparing halloysite ore powder; (2) roughing the halloysite ore; (3) preparing water solutions such as mixed acid and strong-ionicity salt; and (4) carrying out water heating and cleaning at a certain temperature to obtain high-purity halloysite without iron and alunite. According to the high-purity halloysite which is high in purity and free of iron, alunite and similar impurity ores, the step-by-step ion substitution of the alunite is realized, the process cost is low, the alunite and iron impurities generally existing in the halloysite ore can be removed, the purity of the hallosite can be greatly increased, meanwhile, the whiteness of the product is increased, the tubular appearance of the halloysite is not damaged, the internal diameter of a halloysite pipe is properly expanded, and the specific surface area of the product is increased.