Highly c-axis-oriented Ca3Co4-xCuxO9+ (x=0, 0.1, 0.2, and 0.3) thin films were prepared by chemical solution deposition on LaAlO3 (001) single-crystal substrates. X-ray diffraction, field-emission scanning electronic microscopy, X-ray photoelectron spectroscopy, and ultraviolet-visible absorption spectrums were used to characterize the derived thin films. The solubility limit of Cu was found to be less than 0.2, above which [Ca-2(Co0.65Cu0.35)(2)O-4](0.624)CoO2 with quadruplicated rock-salt layers was observed. The electrical resistivity decreased monotonously with increasing Cu-doping content when x0.2, and then slightly increased with further Cu doping. The Seebeck coefficient was enhanced from similar to 100V/K for the undoped thin film to similar to 120V/K for the Cu-doped thin films. The power factor was enhanced for about two times at room temperature by Cu doping, suggesting that Cu-doped Ca3Co4O9+ thin films could be a promising candidate for thermoelectric applications.