Novel uses of higher diamondoids are disclosed. Specifically, higher diamondoids may be used to nucleate diamond films and diamond-like carbon films. Such higher diamondoids include iso-tetramantane [1(2)3], anti-tetramantane [121], the two enantiomers of skew-tetramantane [123], the ten possible pentamantane, the thirty nine possible hexamantanes, the one hundred sixty heptamantanes, as well as the various octamantanes, nonamantanes, decamantanes, and undecamantanes.