More dominant shear flow effect with different shear rates and shear time with assistance of added carbon nanotubes (CNTs) of low amounts on the crystallization kinetics of isotactic polypropylene (iPP) in CNT/iPP nanocomposites was investigated by applying differential scanning calorimetry (DSC), polarized optical microscopy (POM), and rheometer. CNTs were chemically modified to improve the dispersity in the iPP matrix. CNT/iPP nanocomposites with different CNT contents were prepared by solution blending method. The crystallization kinetics for CNT/iPP nanocomposites under the quiescent condition studied by DSC indicates that the addition of CNTs of low amounts significantly accelerates crystallization of iPP due to heterogeneous nucleating effect of CNTs, whereas a saturation effect exists at above a critical CNT content. The shear-induced crystallization behaviors for CNT/iPP nanocomposites studied by POM and rheometry demonstrate the continuously accelerated crystallization kinetics with assistance from added CNTs, with increasing CNT content, shear rate, and shear time, without any saturation effect. The changes of nucleation density for CNT/iPP nanocomposites under different shear conditions can be quantified by using a space-filling modeling from the rheological measurements, and the results illustrate that the combined effects of added CNTs and shear flow on the acceleration of crystallization kinetics are not additive, but synergetic. The mechanisms for the synergetic effect of added CNTs and shear flow are provided.