Thermal analysis, optical and scanning electron microscopy were performed to characterize solution-blended poly(4-methyl styrene) (P4MS)/poly(cyclohexyl methacrylate) (PCHMA) of full compositions. It is concluded that the true state of blend phase structure is miscibility with non-specific intermolecular interactions. To probe molecular interactions between the polymer pairs, FT-IR analysis was also used to assess possible evidence. The FT-IR results for the P4MS/PCHMA suggest that the intermolecular interactions between the pairs are likely non-specific and only comparable with those among the homopolymer molecules. Casting temperature did not seem to have any effect on the miscible phase structure of P4MS/PCHMA. Both optical microscopy and SEM characterization revealed that solution casting of P4MS/PCHMA at either temperature yielded equally homogeneous phase structure. The cloud point phenomenon is attributed to a thermodynamic lower critical solution temperature (LCST) but is kinetically irreversible at normally accessible time scales. The observed LCST could be made to be reversible in an appropriate environment when the molecules were given enough molecular mobility.