Methods of preparing improved settable compositions free of Portland cement and methods of using such compositions in subterranean operations are provided. An example of a method of preparing such compositions may comprise providing an unhydrated mixture of raw materials comprising a silica component, an aluminum component, a magnesium component, a sodium component, a calcium component, a ferrous or ferric component, a sulfurous component, and a potassium component, wherein the mixture has been formed without heating any of the components to above about 3000.degree. F.; and adding water to the unhydrated mixture of raw materials to form a settable composition.