The friction behavior of the nanoscratching process is investigated using molecular dynamic simulations by considering a sphere indenter sliding against a nickel nanofilm structure. In the film/substrate system, the interface-dominated friction process is studied during the nanoscratch process. The results indicate that the interface accommodates deformation during the scratch by absorbing plastic deformation (such as stacking faults and partial dislocations) and by allowing locally interface slip. The observed local material shuffling beneath the tip that was strongly affected by the interface and friction mechanisms, including material ploughing along the track, filling in of the track, and piling up of the chip in front of the tip, are discussed. The combination effects of both scratching depths and film thicknesses were also investigated.