Low-temperature synthesis of polycrystalline germanium (poly-Ge) thin films is of great interest in thin-film photovoltaic and electronics applications. We demonstrate metal (Al)-induced crystallization to form poly-Ge thin films on both glass and polymer substrates at temperatures as low as 200 °C. An interfacial diffusion control layer, intentionally interposed between the Al and the underlying amorphous Ge (a-Ge) layer, is found to achieve layer exchange while suppressing uncontrolled Ge crystallization within the bilayer samples. Germanium thin films with micron-size grains and (111)-preferred orientation are prepared by controlled Ge nucleation and Ge lateral overgrowth of Al during a-Ge crystallization.