This paper builds on prior work exploring the use of risk-associated alternative healthcare (RAAH) in Canada. RAAH uptake was surveyed to explore the characteristics of adult RAAH users and the value of established psychometric instruments previously used in alternative healthcare studies in predicting RAAH behaviours: the Control Beliefs Inventory (CBI), the Reward Responsiveness Behavioural Activation System (RBAS) scale, the Positive Attitudes to Science (PAS) scale, the Satisfaction with Orthodox Medicine (SOM) scale, and the brief version of the Susceptibility to Persuasion-II (StP-II-B) scale. Findings suggest RAAH is influenced by gender, age, income, education, employment, chronic illness status, and ethnicity. Engagement in some form of RAAH was common (around 40%) and the most common types of RAAH use reported were physical manipulation and herbal/nutritional supplement use. Other higher-risk AH activities (such as use of toxins and physically invasive procedures) were also reported by about 5% of respondents. The StP-II-B and PAS instruments were predictive of the likelihood of engagement in RAAH behaviours, as illustrated by higher risk tolerance, desire for novelty, positive attitude to advertising and social influence, and positive beliefs about science. The CBI, RBAS, and SOM instruments were not predictive overall. However, the CBI and SOM instruments were predictive of engagement with physical manipulative RAAH activities, while the RBAS was predictive of herbal/nutritional RAAH engagement. These findings can help inform health professionals’ understanding of public health-seeking behaviours with respect to risk.