The mechanical behavior of semicrystalline isotactic polypropylene (iPP) of different crystallinity, crystal morphology and superstructure was investigated by standard tensile stress-strain analysis, dynamic-mechanical analysis, and in situ observation of the deformation by atomic force microscopy (AFM). Emphasis is put on the comparison of the mechanical characteristics of specimens containing either non-isometric lamellae, being arranged in spherulites, or nodular isometric domains, which are not organized in a superstructure. The formation of lamellae/spherulites and of nodules was controlled by the conditions of crystallization. The replacement of cross-hatched monoclinic lamellae and a spherulitic superstructure by randomly arranged isometric nodules leads to a distinct increase of the ductility and toughness, even if the crystallinity is identical. The modulus of elasticity and the yield stress increase as expected with increasing crystallinity. Slightly lower values of Young's modulus and yield strength are detected if samples contained non-lamellar crystals in a non-spherulitic superstructure, proving an effect of the crystal shape on the deformation behavior. For the first time, tensile deformation of semicrystalline iPP which contains nodular ordered domains instead of lamellae has been followed by in situ AFM.