The research aimed to investigate the molecular dissolution mechanism of both binary and ternary solid dispersions by molecular dynamics simulations. The simulation results indicated that the drug molecules were much easier to be released from surfactant-containing ternary systems than from binary ones. Moreover, sodium dodecyl sulfate as an additive in ternary systems had better effects than Tween 60. The simulation results were in well agreement with the experimental results. This research presented a reasonable explanation of molecular dissolution mechanism for both binary and ternary solid dispersions, which may benefit the future development of solid dispersion formulations.