Oriented mesostructured silica films show potential for the design of nanostructured materials for applications in optics, electronics, and so on. In this report, we propose a new approach to control the orientation of mesochannels using a laser-modified polyimide surface. Pluronic 123 was employed as the structure agent, and mesostructured SBA-15-type silica film was prepared using dip- and spin-coating techniques. The orientation of the mesochannels was evaluated by in-plane X-ray diffraction (XRD) measurements. It was shown that the mesochannels were oriented along the surface microgrooves. The driving force for the orientation of the mesochannels is attributed to the confining effect of the surface microgrooves on the deposited mesochannels.