For the successful development and application of novel lubricant additives, a full understanding of their tribological behaviour at the nanoscale is required, but this can be difficult to obtain experimentally. In this study, nonequilibrium molecular dynamics simulations are used to examine the friction and wear reduction mechanisms of promising carbon nanoparticle friction modifier additives. Specifically, the friction and wear behaviour of carbon nanodiamonds (CNDs) and carbon nano-onions (CNOs) confined between a-iron slabs is probed at a range of coverages, pressures, and sliding velocities. At high coverage and low pressure, the nanoparticles do not indent into the a-iron slabs during sliding, leading to zero wear and a low friction coefficient. At low coverage and high pressure, the nanoparticles indent into, and plough through the slabs during sliding, leading to atomic-scale wear and a much higher friction coefficient. This contribution to the friction coefficient is well predicted by an expression developed for macroscopic indentation by Bowden and Tabor. Even at the highest pressures and lowest coverages simulated, both nanoparticles were able to maintain separation of the opposing slabs and reduce friction by approximately 75 % compared to when no nanoparticle was present, which agrees well with experimental observations. CNO nanoparticles yielded a lower indentation (wear) depth and lower friction coefficients at equal coverage and pressure with respect to CND, making them more attractive friction modifier additives. Potential changes in behaviour on harder and softer surfaces are also discussed, together with the implications that these results have in terms of the application of the studied nanoparticles as lubricants additives.