We have developed a new process to produce ultra-thin crystalline silicon films with thicknesses in the range of 0.1 1 μm on flexible substrates. A crystalline silicon wafer was cleaned by SiF4 plasma exposure and without breaking vacuum, an epitaxial film was grown from SiF4, H2 and Ar gas mixtures at low substrate temperature (Tsub ≈ 200 °C) in a standard RF PECVD reactor. We found that H2 dilution is a key parameter for the growth of high quality epitaxial films and modification of the structural composition of the interface with the c-Si wafer, allowing one to switch from a smooth interface at low hydrogen flow rates to a fragile one, composed of hydrogen-rich micro-cavities, at high hydrogen flow rates. This feature can be advantageously used to separate the epitaxial film from the crystalline Si wafer. As a example demonstration, we show that by depositing a metal film followed by a spin-coated polyimide layer and applying a moderate thermal treatment to the stack, the fragile interface breaks down and allows one to obtain an ultrathin crystalline wafer on the flexible polyimide support.