The preparation and characterization of highly conductive carbon inks is described based on nanocomposites that combine a polystyrene-acrylic resin or water-soluble polymers with a hydrophilic graphene/carbon nanotube hybrid. The water-based carbon inks showed high electrical conductivity and could be effectively used in advanced technologies such as gravure printing for printed electronics. Moreover, the conductivity was shown to be increased with a power law of the nanohybrid volume fraction, with an exponent close to that predicted from the percolation theory, indicating a limited impact of the polymer tunneling barrier on the electrical conductivity of such nanocomposites.