Combinatorial and high-throughput methods can allow for rapid scanning of parameter space for optimization of material properties for applications development. These approaches can also be used to develop fundamental measurements and understanding of problems in materials science. This presentation will illustrate how high-throughput continuous-gradient methods can be applied to problems of polymer-blend phase separation and polymer crystallization. We demonstrate a mapping of the morphology and kinetics of structure evolution in polymer films in two-dimensional composition and temperature sample libraries. Validating control measurements is important to establish a baseline connection to traditional experimentation. The approach will be illustrated in different phase-separating blends, including nanocomposites and nucleated crystallizable thin films, using relatively inexpensive instrumentation.