Halloysite nanotubes (HNTs), a kind of naturally occurring silicates possessing typical fibular structure, were introduced to fabricate polypropylene (PP)/HNTs nanocomposites. The non-isothermal crystallization behaviors were investigated by differential scanning calorimetry (DSC) method according to different treatments. The results suggest, with the inclusion of HNTs in PP matrix, the nanocomposites crystallize at higher temperature regime, which are correlated with the heterogeneous nucleating effects of HNTs during the crystallization process of PP. The kinetics studies of crystallization show that PP nanocomposites possess faster crystallization process and higher activation energy due to the nucleating effect and hindrance effect of HNTs to the motion of PP chains. The polarized light microscopy (PLM) observations further show that HNTs serve as nucleation sites and accelerate the crystallization process.