When applied on the counter electrode of a dye-sensitized solar cell, functionalized graphene sheets with oxygen-containing sites perform comparably to platinum (conversion efficiencies of 5.0 and 5.5%, respectively, at 100 mW cm(-2) AM1.5G simulated light). To interpret the catalytic activity of functionalized graphene sheets toward the reduction of triiodide, we propose a new electrochemical impedance spectroscopy equivalent circuit that matches the observed spectra features to the appropriate phenomena. Using cyclic voltammetry, we also show that tuning our material by increasing the amount of oxygen-containing functional groups can improve its apparent catalytic activity. Furthermore, we demonstrate that a functionalized graphene sheet based ink can serve as a catalytic, flexible, electrically conductive counter electrode material.