Single-crystalline nanostructures of calcium copper titanate, an important giant dielectric quaternary oxide is disclosed for the first time through a convenient molten salt synthesis technique. The technique is not only blessed with high yield but also can readily generate a wide range of morphologies from nanoparticles, nanocubes to nanorods in reproducible way. Most importantly, the as-synthesized nanostructures, irrespective of their shapes, maintain single-crystalline character as it is evident from high-resolution transmission electron microscopic investigation. The present study will pave the way for the development of single-crystalline multi-component perovskite nanostructures which were seem to be extremely hard to realize to date. The possible mechanism on morphological evolution of the as-prepared nanostructures in molten salt is also discussed.