We report here the high-pressure synthesis of well-sintered millimeter-sized bulks of superhard BC 2 N and BC 4 N materials in the form of a nanocrystalline composite with diamond-like amorphous carbon grain boundaries. The nanostructured superhard B-C-N material bulks were synthesized under high P-T conditions from amorphous phases of the ball-milled molar mixtures. The synthetic B-C-N samples were characterized by synchrotron x-ray diffraction, high-resolution transmission electron microscope, electron energy-loss spectra, and indentation hardness measurements. These new high-pressure phases of B-C-N compound have extreme hardnesses, second only to diamond. Comparative studies of the high P-T synthetic products of BC 2 N, BC 4 N, and segregated phases of diamond + cBN composite confirm the existence of the single B-C-N ternary phases.