The structure and properties have been comprehensively studied for metallocene copolymers of propylene-1-hexene (CiPH) and propylene-1-octadecene (CiPOD). The comonomer Content constitutes the most important factor affecting both structure and properties in these CiPH and CiPOD copolymers, although the length of the comonomer is also very important. Thus, a considerable decrease in crystallinity and an easier obtainment of mesomorphic-like ordered entities are observed in the two kinds of copolymers as comonomer content increases. The variations in crystalline structure significantly influence the viscoelastic and mechanical behaviors of these CiPH and CiPOD copolymers. Consequently, the location and intensity of the different relaxation mechanisms as well as stiffness parameters (storage, Young's moduli, and microhardness) and deformation mechanism are strongly dependent upon composition.