We have investigated the thermopower in the organic compound -͑BEDT-TTF͒ 2 RbM͑SCN͒ 4 ͑M =Zn,Co͒ in both its normal and rapidly cooled states. The anomalous temperature dependence of the thermopower is found to extend into the rapidly cooled state and reveals that the charge carriers exhibit both localized and itinerant behaviors. We propose a simple model that captures this feature on the basis of an extended Hubbard model.