Nanostructured coatings of metal (tantalum) containing diamond-like carbon (a-C:Ta) have been prepared by femtosecond pulsed laser deposition (PLD). The films, containing 15 at.% tantalum, have been deposited by ablating sequentially graphite and metallic tantalum in vacuum conditions with an amplified Ti:sapphire laser. The coatings have been investigated by X-ray photoelectron spectroscopy, grazing angle X-ray diffraction, energy filtered transmission electron microscopy, scanning and high resolution transmission electron microscopies. Evidence of metallic α-Ta and β-Ta particles (diameter in the 100 nm range) and smaller quasi-amorphous tantalum clusters embedded in the carbonaceous matrix have been shown. A thin tantalum carbide interface between the carbon matrix and the top surface of the tantalum nodules has also been identified. The ability of femtosecond pulsed laser deposition to synthetize nanocomposite carbon-based films and to control their nanostructure is discussed.