Nickel-titanium shape memory alloys are promising materials in orthopedic applications because of their unique properties. However, for prolonged use in a human body, deterioration of the corrosion resistance of the materials becomes a critical issue because of the increasing possibility of deleterious ions released from the substrate to living tissues. We have investigated the use of nitrogen, acetylene, and oxygen plasma immersion ion implantation (PIII) to improve the corrosion resistance and mechanical properties of the materials. Our results reveal that the corrosion resistance and mechanical properties such as hardness and elastic modulus are significantly enhanced after surface treatment. The release of nickel is drastically reduced as compared with the untreated control. In addition, our in vitro tests show that the plasma-treated surfaces are well tolerated by osteoblasts. Among the three types of samples, the best biological effects are observed on the nitrogen PIII samples.