The first reduction methodology, compatible with flexible, temperature-sensitive substrates, for the production of reduced spin-coated graphene oxide (GO) electrodes is reported. It is based on the use of a laser beam for the in situ, non-thermal, reduction of spin-coated GO films on flexible substrates over a large area. The photoreduction process is one-step, facile, and is rapidly carried out at room temperature in air without affecting the integrity of the graphene lattice or the flexibility of the underlying substrate. Conductive graphene films with a sheet resistance of as low as 700 Ω sq−1 and transmittance of 44% can be obtained, much higher than can be achieved for flexible layers reduced by chemical means. As a proof of concept of our technique, laser-reduced GO (LrGO) films are utilized as transparent electrodes in flexible, bulk heterojunction, organic photovoltaic (OPV) devices, replacing the traditional ITO. The devices displayed a power-conversion efficiency of 1.1%, which is the highest reported so far for OPV device incorporating reduced GO as the transparent electrode. The in situ non-thermal photoreduction of spin-coated GO films creates a new way to produce flexible functional graphene electrodes for a variety of electronic applications in a process that carries substantial promise for industrial implementation.