Hydrogenated amorphous carbon (a-C:H) films are capable of providing excellent superlubricating properties, which have great potential serving as self-lubricating protective layer for mechanical systems in extreme working conditions. However, it is still a huge challenge to develop a-C:H films capable of achieving robust superlubricity state in vacuum. The main obstacle derives from the lack of knowledge on the influencing mechanism of deposition parameters on the films bonding structure and its relation to their self-lubrication performance. Aiming at finding the optimized deposition energy and revealing its influencing mechanism on superlubricity, a series of highly-hydrogenated a-C:H films were synthesized with appropriate ion energy, and systematic tribological experiments and structural characterization were conducted. The results highlight the pivotal role of ion energy on film composition, nanoclustering structure, and bonding state, which determine mechanical properties of highly-hydrogenated a-C:H films and surface passivation ability and hence their superlubricity performance in vacuum. The optimized superlubricity performance with the lowest friction coefficient of 0.006 coupled with the lowest wear rate emerges when the carbon ion energy is just beyond the penetration threshold of subplantation. The combined growth process of surface chemisorption and subsurface implantation is the key for a-C:H films to acquire stiff nanoclustering network and high volume of hydrogen incorporation, which enables a robust near-frictionless sliding surface. These findings can provide a guidance towards a more effective manipulation of self-lubricating a-C:H films for space application.