We present a combined experimental/theoretical study aimed at enhancing adhesion between a NiTi wire and a thermoplastic polyolefin (TPO) matrix in which it is embedded. NiTi wire surfaces were subjected to the following surface treatments prior to pull-out tests: (i)treatment with an acid etch or chemical conversion coating and (ii)application of a surface microgeometry to enhance mechanical interlocking between the wire and the TPO matrix. Nanometer to micron-scale NiTi wire surface features were examined with atomic force microscopy. The extent to which each treatment increased the pull-out force was quantified. Existing theoretical models of wire pull-out based upon strength of materials and linear elastic fracture mechanics are reviewed. Results from a finite element model (FEM), wherein the NiTi/TPO matrix interface is modeled with a cohesive zone model, suggest that the interface behavior strongly depends on the cohesive energy. The FEM model properly accounts for energy dissipation at the debonding front and inelastic deformation in a NiTi wire during pull-out. We demonstrate that residual stresses from the molding process significantly influence mode mixity at the debonding front.