Smoking prevalence amongst service users from the mental health and addictions sectors is higher than the general population. Cross-sectional web- or paper-based surveys comprising open and closed response options were used to examine changes in prevailing attitudes and practices amongst non-government mental health service staff and users. Thematic analysis was used to interpret and present open response answers. Multi-variate logistic models were used to investigate which factors are associated with smoke-free attitudes and practices. Staff who smoke were found to be less likely to provide cessation support to clients (AOR 0.51, 95% CI 0.31–0.82) and gave significantly lower estimates of the percentage of clients who wish to stop smoking (30% vs 44%, p < 0.0001). Those who had completed cessation training also had more positive views about the importance of providing cessation support and service user desire to stop smoking. Staff who had not completed cessation training had significantly lower odds of reporting they carried out quit smoking support often and routinely (AOR 0.33, 95% CI 0.23–0.47) The results suggest that continuing improvement will be enabled by increasing rates of cessation training amongst staff of mental health and addictions non-government organisations. In addition, there is a need for increased incentive and support for staff who smoke to quit.