Shape memory alloys (SMAs), most notably those based on nearequiatomic NiTi, feature distinctive diffusionless phase transformations that give rise to useful functionalities (e.g., to generate force/motion or to store/dissipate deformation energy) that have resulted in wide-scale commercial applications across aerospace, automotive, biomedical, robotics, and other technological fields. [1] Many SMA components feature complex architectures ranging from honeycombs to cellular structures designed to lightweight system components, to match stiffness with adjoined materials, or to intensify deformation responses. [2] Unfortunately, these same phase transformations and resultant thermal-mechanical behaviors that make SMAs desirable also make their manufacture notoriously challenging. NiTi-based SMAs particularly exhibit acute sensitivity to chemistry and microstructure that can be strongly affected by thermal-mechanical histories developed during processing and service. [3] Numerous strategies have been explored to manufacture complex-shaped NiTi SMA components, including various methods for metal joining and metal additive manufacturing. [4,5] While these techniques greatly expand the catalog of accessible SMA architectures for specialized technological applications, such high-temperature processing techniques can have difficulty maintaining precise control over material chemistry. For example, selective laser melting and fusion welding techniques can cause NiTi in localized regions to greatly exceed its melting point (%1310 C), resulting in incongruent volatilization with preferential loss of nickel. The ensuing compositional shift leads to Ti-rich precipitate formation and products whose ductility and shape memory behavior may be significantly impaired. Optimization of processing parameters can reduce the magnitude of these effects, [5] but must be performed on a part-by-part basis. The development of post-processes that can precisely restore the elemental composition of heat-affected material could therefore help enable the wide application of these and other metal manufacturing techniques for NiTi-based SMAs.This work describes a method, SMAs via halide-activated pack equilibration (SHAPE), to manufacture NiTi-based SMAs with precisely controlled chemistries. The SHAPE method improves upon existing reaction-based processing routes employed to synthesize NiTi via solid-state diffusion of titanium into a target substrate. In prior work, drive-in diffusion from a gaseous phase has been accomplished by the use of titanium sponge as a vapor source in the presence of a halide transport agent [6] ; however, titanium cannot be in equilibrium with the desired product NiTi under typical process conditions (i.e., in accordance with the Ni-Ti phase diagram, [7] below 942 C titanium can only be in equilibrium with Ti 2 Ni). Consequently, target substrates in previous studies have been subject to over-titanization resulting in undesired Ti 2 Ni formation and ultimately degrading SMA performance. In the SHAPE method, targe...