Natroalunite is one of colouring minerals in kaolin. In this investigation, natroalunite, on which Ca(II) was adsorbed, was flocculated by HPAM and kaolin was depressed in suspension. The adsorption of Ca(II) on the natroalunite surface was studied by zeta-potential measurement and Auger Electron Spectroscopy analysis. Ca(II) was adsorbed more on the natroalunite surface than on the kaolin surface. The mechanism of Ca(II) adsorption was considered to be chemical adsorption on natroalunite and to be physical adsorption on kaolin. It has been found that Na6P6O18 and Na2Si04 can strongly affect Ca(II) adsorption on the surface of kaolin, but weakly on the surface of natroalunite. The effects of degree of hydrolysis and the molecular weight of HPAM, the effect of pH and the effect of Ca(II) have been studied. The kaolin ore, containing SO3 1.05 per cent has been processed with this method. The products only containing S03 0.36 per cent and the weight ratio of concentrate 52.27 per cent were Obtained.