A general procedure to optimize shape memory alloys (SMAs) for specific engineering performance metrics is outlined and demonstrated through a study of ternary, NiTiX high-temperature SMAs, where X = Pd, Hf, Zr. Transformation strains are calculated using the crystallographic theory of martensite and compared to the cofactor conditions, both requiring only lattice parameters as inputs. Measurements of transformation temperatures and hysteresis provide additional comparisons between microstructural-based and transformation properties. The relationships between microstructural-based properties and engineering performance metrics are then thoroughly explored. Use of this procedure demonstrates that SMAs can be tuned for specific applications using relatively simple, fast, and inexpensive measurements and theoretical calculations. The results also indicate an overall trade-off between compatibility and strains, suggesting that alloys may be optimized for either minimal hysteresis or large transformation strains and work output. However, further analysis of the effects of aging shows that better combinations of uncompromised properties are possible through solid solution strengthening.