Layered phyllosilicates are useful for adsorbing and/or binding to cholesterol and, thereby, reducing blood cholesterol in a patient. Accordingly, provided herein is a method of reducing hypercholesteremia in a mammal comprising administering to the mammal a protonated and at least partially exfoliated layered phyllosilicate material alone and in combination with other cholesterol-reducing agents in an amount effective to reduce hypercholesteremia in the mammal. Also provided are methods of treating a cardiovascular disorder associated with atherosclerosis in a mammalian subject comprising administering to the subject a layered phyllosilicate material in an amount effective to reduce atherosclerotic lesion formation in the subject.