The dynamic vulcanization of reclaimed-tire rubber (RTR) and homopolypropylene (PP) was performed by melt-mixing using either a sulfur crosslinking agent, maleic anhydride (MA), dicumyl peroxide (DCP), or the combination of MA and DCP, in two consecutive machines, first a two-roll mill and then a counterrotating twin-screw extruder. In the case of applying a sulfur crosslinking agent, it was demonstrated that the RTR/PP blend at the ratio of 30/70 had the highest impact strength. This could be attributed to the limitation of carbon black in the blend. When the combination of MA and DCP was applied, the result was higher impact strength of the blend at the same ratio. This could be attributed to not only the cohesion between the polymer chains in each phase, PP phase and rubber phase, but also the interfacial adhesion between PP and RTR chains in these two phases. For comparison, the GRT/PP blends with and without sulfur crosslinking agent were prepared as well. All these blends showed low impact strength, which was nearly the same as that of PP. The effects of different crosslinking agents on dispersion and distribution of rubber domain size, viscosity, and percentage crystallinity were also studied.