Voluntary assisted dying (VAD) is when a terminally ill person with decision-making capacity consensually ends their life with assistance from an authorised professional. Many countries have legalised VAD, and health professionals’ roles within VAD frameworks are varied. Health professionals must be well informed of their legal obligations to ensure they practice within the legal boundaries, and those professionals with objections toward VAD should ensure that their eligible patients have equitable access. Given the current landscape of VAD, it is important to understand different health professionals’ attitudes toward VAD and what may underpin these attitudes. We explored (a) Australian health professionals’ attitudes toward VAD; (b) the psychological components that underpin those attitudes; (c) health professionals’ level of knowledge about VAD; (d) health professionals’ most common beliefs, emotions, and experiences related to VAD. A cross-sectional correlational survey design was used. A total of 182 Australian health professionals participated in the online survey based on a tripartite model of attitudes. We conducted a binomial logistic regression through a Generalised Linear Mixed Model and found polarised attitudes toward VAD between health professionals. Attitudes were accounted for by beliefs, emotions, education, and strength of religious beliefs. Knowledge of VAD was low, but not associated with overall attitude in our model. We highlight the importance of reflexive practice to help health professionals identify their values and feelings related to VAD, and to understand how these may affect their clinical practice. Low knowledge of VAD suggests that legislative and procedural training should be mandatory.