Methods of isolating particular zones within a subterranean formation utilizing self-degrading cement compositions are provided. An example of a method of the present invention is a method that includes: providing a self-degrading cement composition that includes a degradable material, an acid source, a base source, and a water source; placing the self-degrading cement composition in a zone within a subterranean formation; and allowing the self-degrading cement composition to set to form a solid mass that is capable of isolating the zone from a well bore penetrating the zone or from another zone.