Embodiments relate to the use of alkali aluminates and alkali silicates with cement kiln dust to form a settable composition for use in subterranean operations. An embodiment provides a method comprising: introducing a settable composition comprising cement kiln dust, an alkali aluminate, an alkali silicate, and an aqueous carrier fluid into a subterranean formation; and allowing the settable composition to set and thereby reduce fluid flow through a portion of the subterranean formation.