Abstract With a combination of all atom molecular dynamic simulation and experimental study in three neat systems（AO-60/NBR, AO-70/NBR, AO-80/NBR），the objective of this paper is to systematically illustrate the essential mechanism of enhanced damping performance of nitrile-butadiene rubber (NBR) ascribed to the same intense introduction of different hindered phenol. According to the simulation results, AO-80/NBR composite had the largest number of hydrogen bonds, highest binding energy, and smallest fractional free volume, especially with AO-80 content of 97 phr among these three systems, demonstrating the best damping property of the composites than the other systems. In order to better compare with the molecular dynamic simulations, pure mixing rubbers without other additives were used for experimental studying. In anticipation, the MD simulation results were consistent with the following experimental data, which indicate a new attempt theoretical method for predicting the properties of damping rubber material.