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In the present work, two types of novel nano additives, titanium sulfonate ligand/black phosphorus (TiL4/BP) and titanium dioxide/black phosphorus (TiO2/BP) nanocomposites, were prepared. The tribological behavior of the steel/steel friction pairs lubricated by polyalphaolefins type 6 (PAO6) containing the nanocomposites under boundary lubrication was studied. The worn surfaces were analyzed using modern surface techniques. The experimental results show that the rubbed surfaces became smooth and showed little wear with the addition of the nanocomposites. TiO2/BP nanocomposites can significantly improve the lubricity of BP nanosheets under high contact stress. The synergistic roles of the load-bearing abilities and rolling effect of TiO2 nanoparticles, the slip induced by the BP with its layered structure, and the establishment of a tribofilm on the sliding interface are the basis of the tribological mechanisms.