Nanostructures of microwave dielectric (Ba,Sr)TiO3 were prepared by a chemical solution decomposition route and a template assisted sol-gel route respectively. The two dimensional nanostructures exhibited a uniform and nearly monodispersed size, which was a strong function of the substrate. There seemed to be a mixture of particles with different orientations that was present in the thicker films also. The three-dimensional self-assembly showed interesting structures with promising optical characteristics.