In this article we describe the development of the Chemistry Attitudes and Experiences Questionnaire (CAEQ) that measures first-year university chemistry students' attitude toward chemistry, chemistry self-efficacy, and learning experiences. The instrument was developed as part of a larger study and sought to fulfill a need for an instrument to investigate factors that influence student enrollment choice. We set out to design the instrument in a manner that would maximize construct validity. The CAEQ was piloted with a cohort of science and technology students (n = 129) at the end of their first year. Based on statistical analysis the instrument was modified and subsequently administered on two occasions at two tertiary institutions (n = 669). Statistical data along with additional data gathered from interviews suggest that the CAEQ possesses good construct validity and will prove a useful tool for tertiary level educators who wish to gain an understanding of factors that influence student choice of chemistry enrolment. © 2003 Wiley Periodicals, Inc. J Res Sci Teach 40: 649–668, 2003