A structure designed to show functionality on the nanometer length scale ideally would spontaneously form periodic nanometer-scale patterns comprising regions with contrasting properties. Here we report the synthesis of three new oxides that spontaneously form a variety of nanostructures with a periodic arrangement of phases with compositional and functional contrast. This is achieved through the partial substitution of Ti by Al, Cr, and Mn in periodically phase-separated (Nd2/3-xLi3x)TiO3 nanochessboard structures. The generality of this spontaneous compositional nanopatterning is promising for an array of exotic bulk and nanostructural properties.