Phosphazene-silicate nanocomposites were synthesized and their mechanical properties analyzed. Three distinct types of catalysts were employed to drive the ceramic condensation - acid, base and ionic salt species - resulting in a wide variety of mechanical properties. To validate the correlations between the physical properties observed and the ceramic morphologies formed, a survey of the extent of parent polymer degradation under these catalytic conditions was undertaken. Further, the effects of various ionic strengths of casting solutions resulting from relative dissociation constants, hence active catalyst availability, on salt-catalyzed silicate interpenetrating network (IPN) matrices were also investigated. The resulting information provides the appropriate synthetic control needed to produce nanocomposites with specifically tailored properties for a variety of applications.