Methods of fabricating high-k dielectric layers having reduced impurities for use in semiconductor applications are disclosed. The methods include the steps of: forming a stacked dielectric layer having a first dielectric layer and a second dielectric layer formed on a semiconductor substrate using an ALD method, in combination with a post-treatment step performed to the stacked dielectric layer. The steps of forming the stacked dielectric layer and performing the post-treatment are repeated at least once, thereby fabricating the high-k dielectric layer.