Controlling droplet deposition with a minute amount of polymer additives is of profound practical importance in a wild range of applications. Previous work ascribed the relevant mechanisms to extensional viscosity, normal stress, wetting properties, etc., but the mechanism remains controversial. In this paper, we employ molecular dynamics simulations systematically for the first time to investigate the origin of rebound suppression for dilute polymer solution droplets on a flat superhydrophobic substrate. The results demonstrate that polymer−substrate interactions and impact velocities dominate the antirebound phenomenon. For low impact velocities, the dynamic characteristics of droplets are insensitive to polymer additives. However, large impact velocities will enhance the stretch behavior of polymer chains and make the chains closer to the substrate, increasing the probability of polymer molecules contacting the bottom substrate. With the cooperation of strong polymer−substrate interactions, polymer molecules can be absorbed easily by the bottom substrate, resisting the retraction process and leading to the onset of the antirebound behavior.