Shape memory alloys (SMAs) have gained attention in recent years as a powerful mechanism for mechanical actuation in space applications. One issue facing this technology is that most commercially available SMAs yield a high amount of energy loss due to their relatively large hysteresis, which can translate into an increase in the overall cost of the mission. Low hysteresis shape memory alloys (LHSMAs), which exhibit a much narrower hysteresis, are needed to minimize this energy loss. Previous studies have shown that elemental additions of Cu, Co, and Pd to the NiTi-based SMA can result in shape memory alloys with a much lower thermal hysteresis, due to better phase compatibility. This present work investigated seven alloy compositions to identify LHSMAs with less than 20 °C hysteresis and develop processing routes for these LHSMAs to determine potential candidates for space actuation applications.