Sr2TMO3 (TM = Ni,Co) compounds with 1D TM-O chains have been successfully synthesized in the form of single-crystalline thin films using a combinatorial approach. The crystal structure is examined using X-ray diffraction and high-resolution TEM (see figure). Polarized absorption spectroscopy and third-harmonic generation spectroscopy reveal a 1D electronic structure and sizable nonlinear optical susceptibility, respectively, for Sr2NiO3.