Investigations of nanocar motion on one-dimensional substrate surfaces provide an important contribution to the practical goal of designing nanoscale transporters. As a preliminary step toward modeling the dynamics of these species, first-principles vdW-DF calculations were performed to investigate the interaction between the nanocar and the graphene/graphyne surface. The accuracy of this method is validated by experimental results and the MP2 level of theory. The results obtained reveal that the nanocar would require at least −71.39 and −18.33 kJ mol−1 to activate its movement on the graphene and graphyne surfaces, respectively. First-principles molecular dynamics simulations show that the nanocar moved on the substrate without additional external factors under ambient conditions. The nanocar displays a tendency toward slipping on the graphyne surface within 2 ps of simulation time movement. These findings provide insights that will facilitate the coherent design and control of surface-operational molecular
