Combinatorial libraries of segmented polyurethaneurea with gradients in curing temperature were prepared and characterized using a novel high‐throughput mechanical instrument. Stress/strain profiles were taken at different temperature positions on the libraries, and a structure/property relationship between microstructure and mechanical properties was established by correlating the measured strength and strain at break to high‐throughput AFM and FT‐IR measurements on the same library. These results demonstrate the feasibility of rapid and accurate screening of mechanical properties, and their correlation to structure, by using gradient combinatorial polymer libraries.