Nanodiamond (ND) particles are effective lubricant additives. Attention of research has shifted towards investigating the particles as secondary additives. ND particles provide more benefits as secondary additives than as the sole lubricant additive for steel–steel contacts. In this work, the influence of ND particles as secondary additives on oil lubrication of steel–aluminium tribopair (hard–soft contact) was examined. AISI 52100 steel balls were slid against AA2024 aluminium alloy discs, in the presence of polyalphaolefin (PAO) base oil, in boundary lubrication regime (applied normal load: 10 N to 50 N). Primary additives were copper oxide (CuO) and hexagonal boron nitride (h-BN) nanoparticles. The addition of ND particles to PAO, with CuO and h-BN as primary additives, at the lowest applied normal load of 10 N: (i) decreased the volumetric wear of the aluminium discs by 28% and 63%, respectively, and (ii) decreased the coefficient of friction by 15% and 33%, respectively. At the highest applied normal load of 50 N, it: (i) decreased the volumetric wear of the aluminium discs by 20% and 38%, respectively, and (ii) decreased the coefficient of friction by 5.4% and 8%, respectively. ND particles as secondary additives significantly reduce energy loss and power loss as a consequence of an effective reduction in friction during sliding. Unique characteristics of ND particles—such as their (a) physicochemical and thermal properties, (b) ball bearing and polishing effects and (c) synergistic interaction with primary additives to form stable tribofilms—enhance the lubrication performance of steel–aluminium contact. ND particles in combination with h-BN nanoparticles showed the best performance, due to better synergy between the primary additive and the secondary additive. Results from the investigation indicate that ND particles taken as secondary additives in small amount (0.2 wt%) can improve oil lubrication performance of hard–soft contacts in engineering systems.