The current study was undertaken to investigate the synthesis of CrAlN/BN composite coatings having super high hardness by a reactive co-sputtering using CrAl alloy and BN targets and gaseous mixture of Ar+N2, in order to eliminate the possible formation of boride bonding. CrAlN or BN phase was deposited by pulsed d.c.- and r.f.- sputtering, respectively. Plastic hardness, Hpl, and Young’s modulus, E*, of the coatings increased with BN phase ratio, reaching a maximum value of ~46 GPa and 390 GPa at ~8 vol. % of BN phase; and then decreased to ~20GPa and ~300GPa at ~18 vol.%, respectively. Only B1 structured Cr(Al)N phase was found in XRD and SAED analysis. XPS and TEM/HRTEM results revealed that the CrAlN/8vol%BN coating consists mostly of CrAlN and BN phase, which exists as an amorphous like phase among the CrAlN grains. The CrAlN/8vol%BN coating has a kind of nanocomposite structure and the super high hardness over 40 GPa is probably due to this structure.