A nematic liquid crystalline polysiloxane has been found to be a novel nucleating agent (LCP-NA2) to induce the formation of beta-crystals in isotactic polypropylene (iPP). Wide angle X-ray diffraction, differential scanning calorimetry, and polarized optical microscopy were used to evaluate the nucleating activity of LCP-NA2. The effect of LCP-NA2 content, crystallization temperature, and time on the crystallization structure, morphology, and thermal behavior of the iPP was discussed. The results indicated that the nucleating activity mainly depended on LCP-NA2 content and thermal history of processing. The addition of LCP-NA2 could provide a large number of nuclei and lead to a more uniform morphology, along with a change in the nucleation and crystal growth mechanism. The relative content of beta-crystal increased with increasing LCP-NA2 content or crystallization temperature, reached a maximum value of 70 % when LCP-NA2 content and crystallization temperature were 1.0 wt% and 125 A degrees C, and then decreased with a further increase of LCP-NA2 content or crystallization temperature. In addition, a different polymorphic behavior had been observed between pure iPP and LCP-NA2/iPP blends under the same thermal treatment.