Thermoelectric (TE) technology attracts much attention due to the fact it can convert thermal energy into electricity and vice versa. Thin-film TE materials can be synthesized on different kinds of substrates, which offer the possibility of the control of microstructure and composition to higher TE power, as well as the development of novel TE devices meeting flexible and miniature requirements. In this work, we use magnetron sputtering to deposit N-type and P-type BiTe-based thin films on silicon, glass, and Kapton HN polyimide foil. Their morphology, microstructure, and phase constituents are studied by SEM/EDX, XRD, and TEM. The electrical conductivity, thermal conductivity, and Seebeck coefficient of the thin film are measured by a special in-plane advanced test system. The output of electrical power (open-circuit voltage and electric current) of the thin film is measured by an in-house apparatus at different temperature gradient. The impact of deposition parameters and the thickness, width, and length of the thin film on the power output are also investigated for optimizing the thin-film flexible TE device to harvest thermal energy.