The spherulitic superstructure, crystallinity, and structure and morphology of crystals of isotactic polypropylene were controlled by the conditions of melt crystallization and related to the transmittance of visible light. Spherulitic samples, which contained monoclinic lamellae, were prepared by slow cooling of the quiescent melt at rates lower than 10 K/s and by isothermal melt crystallization at temperatures between 373 and 413 K. Nonspherulitic specimens, which contained nonlamellar mesomorphic domains, in contrast, were obtained by rapid cooling of the melt with rates faster than 100 K/s. The crystallinity and the size of crystals were furthermore fine-tuned by subsequent annealing at elevated temperatures. Analysis of such films of different structure by ultraviolet-visible spectroscopy revealed that the light transmission was independent of (1) the fraction, (2) the internal structure, and (3) the size of the crystals. In contrast, the light transmission increased with decreasing size of spherulites and finally exceeded 90% in films of 100 lm thickness when spherulites were completely absent. The crystallinity and the structure and size of the crystals of the films of isotactic polypropylene could be adjusted within wide limits without affecting the light transmission.