Reactive extrusion of polypropylene (PP)/natural rubber (NR) (90/10) blends was conducted in the presence of a peroxide[1,3-bis(t-butylperoxy)benzene] and coagent (trimethylolpropanetriacrylate, TMPTA). Effects of peroxide and coagent content were studied in terms of melt index (MI), melt viscosity, morphology, thermal, and mechanical properties. At a constant content of the coagent, melt viscosity increased at a low and decreased at a high content of the peroxide. On the other hand, melt viscosity increased monotonically with the coagent concentration at constant peroxide content. The increase and decrease of viscosity were interpreted in terms of crosslinking and chain scission of PP, which governed the rubber domain size and mechanical properties of the reactive blends.