Shape memory and superelastic applications of NiTi based alloys have typically been limited to near room temperature or to bulk length scales. The objective of this work is two-fold: first, to investigate shape memory behavior at low temperatures in the context of the R-phase transformation in NiTiFe alloys by recourse to arc-melting, differential scanning calorimetry (DSC), transmission electron microscopy (TEM) and mechanical testing at low temperatures; and second, to investigate superelasticity and two-way shape memory behavior at reduced length scales in the context of NiTi by recourse to micro-compression, micro-indentation and TEM studies. Selected compositions of ternary NiTiFe shape memory alloys were arc-melted and thermomechanically processed to investigate the influence of composition and processing parameters on the formation of the R-phase. The methodology used for the processing and characterization of the alloys was established and included microprobe analysis, DSC, TEM and mechanical testing. No phase transformation was observed in alloys with Fe content in excess of 4 at.%. Thermomechanical treatments facilitated the formation of the R-phase in Ni-rich alloys. The range of the transformation between the R-phase and austenite, and the hysteresis associated with it were influenced by the distribution and size of metastable Ni4Ti3 precipitates. The investigation of the microstructural, thermal and mechanical properties of the R-phase transformation in NiTiFe alloys revealed a complex dependence of these properties on processing parameters. The present work also highlighted the hitherto unexplored competition between the two inelastic deformation modes operating in the R-phase (detwinning and stress-induced transformation) and established the preference of one mode over the other in stress-temperature space. iv The complete micromechanical response of superelastic NiTi was examined by performing careful micro-compression experiments on single crystal pillars of known orientations using a nanoindenter tip. Specifically, the orientation dependence of the elastic deformation of austenite, the onset of its transformation to martensite, the gradient and the hysteresis in the stress-strain response during transformation, the elastic modulus of the stress-induced martensite and the onset of plasticity of the stress-induced martensite were analyzed in separate experiments. A majority of the results were explained by recourse to a quantitative determination of strains associated with austenite grains transforming to martensite variants or twinning in martensite. Microstructural studies were also performed on a micro-indentation trained NiTi shape memory alloy specimen to understand the mechanisms governing the two-way shape memory effect. In situ TEM studies at temperature on specimens obtained at different depths below the indent showed the presence of retained martensite along with the R-phase. Previously, while such twoway shape memory behavior has typically been associated with large dislocation densities, this work provides evidence of the role of retained martensite and the R-phase in cases with reduced dislocation densities. Funding support for this work from NSF (CAREER DMR-0239512), NASA (NAG3-2751) and SRI is acknowledged.