Cosmetic compositions capable of forming a multilayer structure after application to a keratinous material are provided, as well as methods of applying such compositions to a keratinous material. Certain cosmetic compositions comprises at least two immiscible components: Component A which comprises about 0.01% to 60% by weight with respect to the total weight of the composition of at least one hydrocarbon-containing film forming agent having at least one glass transition temperature which is lower than normal human body temperature; and Component B which comprises about 0.01% to 90% by weight with respect to the total weight of the composition of one or more silicone compounds in amounts sufficient to achieve a viscosity of about 1,000 cSt to 10,000,000 cST, wherein the weight ratio of hydrocarbon-containing film forming agent(s) in Component A to silicone compound(s) in Component B is from about 1:50 to 50:1.