Nitrile butadiene rubber (NBR) and its various composite materials are widely employed as friction materials in mechanical equipment. The use of carbon nanotube (CNT) reinforcement in NBR for improved friction and wear characteristics has become a major research focus. However, the mechanisms underlying the improvement in the friction and wear characteristics of NBR with different CNT contents remain insufficiently elucidated. Therefore, we conducted a combined analysis of NBR reinforced with varying CNT contents through molecular dynamics (MD) simulations and ring–block friction experiments. The aim is to analyze the extent to which CNTs enhance the water-lubricated friction and dry wear properties of NBR and explore the improvement mechanisms through molecular chain characteristics. The results of this study demonstrate that as the mass fraction of CNTs (0%, 1.25%, 2.5%, 5%) increases, the water-lubricated friction coefficient of NBR continuously decreases. Under water-lubricated conditions, CNTs improve the water storage capacity of the NBR surface and enhance lubrication efficiency. In the dry wear state, CNTs help reduce scratch depth and dry wear volume.