The phase structure and dynamic mechanical properties of three polypropylene/polystyrene (PP/PS) systems of similar composition but various dispersion of the minor PS component have been examined. Two different PP/PS systems were prepared by polymerization of styrene (ST) molecularly dispersed in PP matrices (with the same initial structure) under the conditions leading to a linear or crosslinked PS component. The third PP/PS system has been prepared blending the homopolymers in the molten state. Studies of materials containingin situ polymerized PS revealed nanoscale phase separation of PS (atomic force microscopy) and pointed to the presence of physical entanglements between PS and non-crystalline phase of PP (DSC, dynamic mechanical analysis). The PS component in material prepared by melt mixing appeared to be completely phase-separated into micron-sized domains. Dynamic mechanical analysis revealed also the dependence of viscoelastic behavior of the PP/PS systems on dispersion of the PS inclusions and on the nature of the interface.