We extended prior voluntary turnover research by investigating the relationships between boundaryless career attitudes and voluntary turnover. Specifically, we explored whether boundaryless career attitudes are widely held, and if such attitudes contribute to voluntary turnover behaviors. To answer the questions, we developed a scale measuring boundaryless career by adopting Ajzen’s theory of planned behavior, Betz et al.’s career decision making scale, and Bandura’s self-efficacy concept. The survey from 303 undergraduates in Hong Kong showed the instrument’s reliability and validity are acceptable. Exploratory factor analysis supported our theorizing that boundaryless career orientation consists of individual’s attitude, subjective norm and perceived behavioral control. Correlational analysis implied that boundaryless career attitudes are widespread, and such attitudes could contribute to voluntary turnover behaviors.