Carbon nanotubes have been explored to increase the mechanical properties and electrical conductivity of polymeric fibers through compounding with polymer to be extruded into fibers. However, this route creates major challenges because carbon nanotubes have strong cohesion and tend to aggregate and precipitate due to their poor interfacial interaction with polymers. In this study, classical molecular dynamics simulations are used to predict and characterize carbon nanotubes-polymer interface mechanism in two different polymer matrices: polyvinyl butyral and polystyrene-co-glycidyl methacrylate. The dominated interface mechanisms are discovered to shed light on carbon nanotubes dispersion in solvent based systems and to explore the prerequisites for stabilized nanofluids. Our results showed that π-stacking interactions between aromatic groups and graphene surfaces of carbon nanotubes as in polystyrene-co-glycidyl methacrylate systems, play an important role in dispersion of carbon nanotubes, whereas slight repulsions between carbon nanotubes and polyvinyl butyral chains lead to large morphological differences and carbon nanotubes bundles in many chain systems. Altogether, the results indicated that polymers with structures having strong interactions with the surfaces of carbon nanotubes through π–π interactions are more effective in dispersing carbon nanotubes and caused stabilized solutions in wet fiber processing.