Poly(p-phenylene terephthalamide) (PPTA)/amorphous nylon (AN) molecular composites were prepared from sulfuric acid solution by rapidly coagulating in distilled water. The regenerated films appear homogeneous and transparent. However, the rod-like and flexible macromolecules are probably entrapped in a single phase during rapid coagulation, thus thermodynamically unstable and undergoing phase segregation upon thermal treatment. The miscibility between PPTA/AN was identified by a dielectric relaxation method. Phase behavior and kinetics of phase separation in PPTA/AN mixtures were thoroughly investigated by time-resolved light scattering as well as optical microscope. A pseudo phase diagram reminiscent of a lower critical solution temperature (LCST) was established by a cloud point measurement. Several temperature-jump experiments were undertaken from ambient to a two-phase temperature region. The low PPTA content molecular composites were prepared by coagulating in a non-solvent, then by compression molding below the phase separation temperatures. The 30 wt% PPTA molecular composite exhibits over three-fold increase in tensile modulus relative to that of the neat AN, however, there is little or no improvement in the tensile strength. On the other hand, by a slight addition of AN into PPTA, the tensile and compressive failures of spun fibers may be improved.