Amorphous carbon film, which combines good chemical inertia, wear resistance and mechanical properties, has been applied in aerospace, automotive, magnetic storage, mechanical processing and other fields. sp3 ratio and H content significantly influence microstructure and tribological properties of amorphous carbon. Especially, the tribological behavior of amorphous carbon with different sp3 ratio and H content varies greatly in the run-in stage under vacuum and air, which means a lot for wear pair design in aerospace equipment components. This work aims to investigate the relationship between film structure and properties, so as to find the optimum processing window.