Nanoimprint templates made of diamond-like carbon (DLC) and amorphous silicon carbide (SiC) thin films and fluorine-doped associated materials, i.e. F-DLC and F-SiC were investigated in the context of thermal nanoimprint lithography (NIL) with respect to their release properties. Their performances in terms of durability and stability were evaluated and compared to those of conventional silicon or silica molds coated with antisticking molecules applied as a self-assembled monolayer. Plasma-enhanced chemical vapor deposition parameters were firstly tuned to optimize mechanical and structural properties of the DLC and SiC thin films. The impact of the amount of fluorine dopant on the deposited thin films properties was then analyzed. A comparative analysis of DLC, F-DLC as well as SiC and F-SiC molds was then carried out over multiple imprints, performed into poly (methyl methacrylate) (PMMA) thermo-plastic resist. The release properties of un-patterned films were evaluated by the measurement of demolding energies and surface energies, associated with a systematic analysis of the mold surface contamination. These analyses showed that the developed materials behave as intrinsically easy-demolding and contamination-free molds over series of up to 40 imprints. To our knowledge, it is the first time that such a large number of imprints has been considered within an exhaustive comparative study of materials for NIL. Finally, the developed materials went through standard e-beam lithography and plasma etching processes to obtain nanoscale-patterned templates. The replicas of those patterned molds, imprinted into PMMA, were shown to be of high fidelity and good stability after several imprints.