The synthesis and preparation of a new type of graphene composite material suitable for spin-coating into conductive, transparent, and flexible thin film electrodes in ambient conditions is reported here for the first time. Solution-processible graphene with diameter up to 50 μm is synthesized by surfactant-assisted exfoliation of graphite oxide and in situ chemical reduction in a large quantity. Spin-coating the mixing solution of surfactant-functionalized graphene and PEDOT:PSS yields the graphene composite electrode (GCE) without the need for high temperature annealing, chemical vapor deposition, or any additional transfer-printing process. The conductivity and transparency of GCE are at the same level as those of an indium tin oxide (ITO) electrode. Importantly, it exhibits high stability (both mechanical and electrical) in bending tests of at least 1000 cycles. The performance of organic light-emitting diodes based on a GCE anode is comparable, if not superior, to that of OLEDs made with an ITO anode.