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Poly(chloroprene) is a synthetic crystallizable polymer used in several applications, including rubber gloves. The film formation of poly(chloroprene) latex offers opportunities to define structures at length scales between the molecular and macroscopic, thereby adjusting the elastomer’s mechanical properties. However, the connections between processing and the resultant film properties are not fully understood. Here, we investigate the competition between the coalescence of latex particles to build cohesive strength and their crystallization to raise the elastic modulus. We demonstrate that when coalescence precedescrystallization, the elastomer has greater extensibility and a higher tensile strength compared to when crystallization occurs duringcoalescence. The mechanical properties of poly(chloroprene) were tuned by blending two colloids with differing gel contents and crystallizabilities. Heating above poly(chloroprene)’s melting temperature allows increased particle interdiffusion and builds cohesion, prior to recrystallization. We provide evidence from in situwide-angle X-ray scattering for the strain-induced crystallization of as-cast films from particle blends.