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In this study, willow catkins/MoS2 nanoparticles (denoted as WCMSs) have been prepared using a hydrothermal method. The WCMSs were modified with oleic acid (OA) to improve dispersion in base oil. The friction and wear properties of WCMSs in liquid paraffin (LP) for steel balls were investigated using a four-ball wear tester. The results have shown that at a high reaction temperature, willow catkins (being used as a template) and urea (being used as a nitrogen resource) can effectively decrease the wear scar diameters (WSDs) and coefficients of friction (COFs). At a concentration of 0.5 wt.%, the WSD and COF of steel balls, when lubricated using LP containing modified WCMS with urea, decreased from 0.65 mm and 0.175 of pure LP to 0.46 mm and 0.09, respectively. The addition of urea and hydroxylated catkins can generate a significant number of loose nano-sheets and even graphene-like sheets. The weak van der Waals forces, decreasing the shear forces that the steel balls must overcome, provide effective lubrication during rotation. On the other hand, the tribo-films containing MoS2, FeS, azide, metal oxides and other compounds play important roles in reducing friction and facilitating anti-wear properties.