LDPE/PP polyblends, modified through either peroxide initiated reactions or irradiation, were characterized in terms of rheological and mechanical properties and microstructure. In the presence of peroxide, or through irradiation LDPE crosslinks, PP degrades. Data were obtained at two peroxide concentration levels (0.1 and 1% by weight) and two radiation doses (30 and 100 kGy). The results show that in peroxide modification, the degradation of PP prevails over the crosslinking of LDPE. However, the effect of irradiation on LDPE (crosslinking) is predominant over that of PP (degradation). The irradiation process tends to yield improved mechanical properties vs. peroxide modification for the PP-rich blends. In addition, the melt viscosity and elasticity of the irradiated PP-rich blends are higher than those of the peroxide-reacted blends at a given level of PP content and frequencies between 10 and 100 rad/s. Attempts were made to relate the shape of the rheological curves and the mechanical properties of the blends to the observed changes in their microstructure.