For the discovery and optimization of high temperature shape memory alloys (HTSMA) combinatorial and high-throughput thin film experimentation methods are applied. HTSMAs are deposited as thin film materials libraries by combinatorial sputtering. The obtained materials libraries are measured by high-throughput characterization methods in order to correlate compositional data with structural and functional properties. Results are visualized as composition-structure-function diagrams (functional phase diagrams). This contribution discusses results which were obtained by this approach in Ti-Ta-X and Co-Ni-X-Y materials systems, involving the quantitative mapping of phase transformation properties in the identified composition ranges.