A zinc salt of a lightly sulfonated (4.5 mol %) polystyrene ionomer was used to compatibilize a 3/1 (w/w) blend of syndiotactic polystyrene and a wholly aromatic thermotropic liquid-crystalline polymer (TLCP). The addition of the ionomer significantly reduced the dispersed TLCP domain size and improved the tensile strength, ultimate elongation, and flexural toughness of the blend.