Microprocessable materials, or materials processable on the micrometer scale, are the key to progress in nanotechnology. Research on photofunctional soft organic materials is an increasingly important area because of their processability and flexibility, which are advantageous to of photonic device systems.[1±7] Thin films of azobenzene-containing polymers (azopolymers) are interesting materials because of their ability to self-organize into structures on the micrometer and nanometer scales, assisted by light. [8] These structures are called photoinduced surface reliefs, and are attributed to mass transport over micrometer distances during trans±cis photoisomerization. [9][10][11][12][13][14] When a flat azopolymer film is exposed to interfering coherent light at an absorption wavelength, a surface relief grating (SRG), i.e., a regular surface relief modulation identical to the interference pattern in a grating period, is formed on it. Once formed, the SRG is stable as long as the polymer is kept in the dark below the glass-transition temperature. However, the SRG can be erased by heating or upon exposure to uniform light at the appropriate absorption wavelength, and can be formed again by exposure to an interference pattern. Taking advantage of these features, we expected that azopolymers could be used in dynamic devices, such as a wavelength-programmable organic distributed-feedback (DFB) laser in which optical feedback is provided by the periodic modulation of either the refractive index or the optical gain, or both.[15±26]Although a few researchers have reported on DFB lasers based on azopolymers with photoinduced SRGs, the SRGs were used only as templates for the grating. [25,26] As yet, there are no reports on the advantages of SRGs formed on azopolymers in terms of their erasable and rewritable properties. In this study, we demonstrate organic DFB lasers with wavelength programmability by utilizing the advantages of SRGs, i.e., the grating can be erased and rewritten. In the design of organic DFB waveguide lasers, single lateralmode propagation, sufficient optical gain, and Bragg diffraction are necessary to obtain a single-peak laser output spectrum. We first attempted to realize a DFB laser using a dye-doped azopolymer film with an SRG. However, the fluorescence of all the laser dyes investigated was significantly quenched, so that the optical gain of the doped film was insufficient for lasing. This quenching was attributed to electron transfer from the azobenzene to the laser dye. To prevent this, we designed a double-layered DFB laser composed of a diffraction layer of an azopolymer, poly{(4-nitrophenyl) [4-[[2-(methacryloyloxy)ethyl]ethylamino]phenyl]diazene}, (pDR1M), and an active layer of laser-dye-doped poly(vinyl alcohol) (PVA) on a synthetic quartz substrate. We employed malachite green (MG) and sulforhodamine (SR) as laser dyes. By placing the azopolymer layer on the top of the active layer, the azopolymer layer had a free surface which enabled us to construct, erase, and rewrite SRGs.The refra...