A high-melt-strength polypropylene (HMSPP) with partially cross-linking, modified from a normal isotactic polypropylene (IPP), is prepared by a one-step silane grafting and cross-linking method in a twin-screw reactive extruder. The melt grafting and cross-linking of IPP is achieved by using vinyl unsaturated silane with long chain as a grafting monomer, benzoyl peroxide (BPO) as an initiator, styrene as a coagent, and a little water as a catalyst for cross-linking. By analyzing the difference of the Fourier transformed infrared spectra between raw and modified PP, comparing the variety of the melt flow rate (MFR) and gel percentage between cured and uncured PP samples, and investigating the effect of catalyst on the MFR and gel percentage of modified PP, the partially cross-linked polypropylene in the way of one-step reactive extrusion has been verified. We put forward the reactive mechanism of one-step method based on our experimental results. In this mechanism, the hydrolysis and condensation of silane occur first through the catalysis of water and a compound with two or more double-bond is formed, which then the compound reacts with PP macroradicals to form the partially cross-linked PP.