This study covers the preparation of noncrosslinked and crosslinked solvent-cast blend films of ultrahigh molecular weight polyethylene (UHMWPE) and polyisoprene rubber (PIR) and their mechanical, thermal, IR spectroscopic, and morphological characterizations. Solvent-cast films of polymer blends with 0, 10, 20, 35, 50, and 65% PIR composition were prepared by vigorous stirring from a hot decalin solution. The films were crosslinked chemically by using acetophenone as a crosslinking agent under UV radiation. The mechanical properties, measured as ultimate properties and tensile modulus, were found to decrease with PIR content but crosslinking was found to enhance the ultimate strength and tensile modulus. DSC results revealed that melting point of UHMWPE remains almost constant in blends. However, upon crosslinking, the melting point of UHMWPE is depressed almost 5 degrees C. We observed a similar trend in the enthalpy change of the melting of UHMWPE and the variation of percent crystallinity in UHMWPE. Scanning electron microscopy (SEM) studies on the fractured surfaces of the blends showed that the fibrillar texture is present in both crosslinked and noncrosslinked blends. The crosslinking appeared to be through oxygen linkages, which are preferentially conjugated to double bonds, in addition to the possible carbon-carbon crosslinks.