A novel polymer-based optoelectronic device is created to independently realize either photoelectric conversion or light emission. It is produced by coating photoactive materials on one side of an aligned carbon nanotube sheet electrode and polymer light-emitting materials on the other side of the carbon nanotube sheet electrode through an all-solution process. The power conversion efficiency exceeds 2% and the brightness reaches 1040 cd/m2 for photoelectric conversion and light emission parts, respectively. This work indicates a promising potential for a wide variety of applications including micro-electronic, smart and multi-function devices through all-solution-based processes.