Disclosed are a variety of self-supporting, multilayer carbon films that include a layer of both a non-diamond-like carbon, for example, graphitic or amorphous carbon (or a-C), and a layer of diamond-like carbon (DLC). A wide range of multilayer configurations may be constructed depending on the particular combination of properties desired in the final product including, for example, a tri-layer construction including a single DLC layer sandwiched between two layers of amorphous carbon. Also disclosed are example embodiments of methods for producing such composite multilayer films that include preparing an appropriate substrate to include a deposition surface of sufficient smoothness, applying a parting or release agent to the deposition surface, depositing a plurality of layer carbon layers including both an amorphous carbon layer and a DLC layer to form the composite carbon film and removing the composite carbon film from the substrate.