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Teacher entrepreneurial behavior (TEB) enables teachers to seize innovation opportunities and scale-up innovation in schools. However, the present lack of a well-validated TEB measure not only inhibits research progress on TEB, but it also threatens the adequacy of findings related to TEB. The present paper describes our effort to develop a valid TEB scale. We drew on existing empirical TEB research, especially a recent conceptual TEB framework proposed by Authors (2021), and conducted four interconnected studies by following scale-development procedures. We developed and tested a four-dimension scale of TEB and found that it significantly predicts key teacher outcomes, including job satisfaction, team trust, and school innovation.