A series traditional thermoelectric films, including n-type Bi, Bi2Te3, and p-type Sb, Sb2Te3, were synthesized with CH3NH3I by combining magnetron sputtering and thermal evaporation method. It is found that the Seebeck coefficients for all the composite films have enhanced although the electrical conductivities reduced due to the decreased carrier concentration. This leads to an obvious improvement of the power factor, especially for p-type Sb2Te3-based organic-inorganic hybrid films. As expected, a maximum power factor value around 2.3mWm(-1)K(-2) has been achieved for the composition of Sb2Te3/CH3NH3I in range of the whole measured temperature, which is nearly seven times higher than that of pristine Sb2Te3 film. By combination with the reduced thermal conductivity, a ZT value nearly 1.0 has been obtained at 380K for the composition of Sb2Te3/CH3NH3I.