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Accessible Summary: What is known on the subject?: People diagnosed with serious mental illness have a high risk of diabetes and are more likely to develop type 2 diabetes at ages below 60 years.Effective diabetes self‐care behaviours among people diagnosed with serious mental illness can improve glycaemic control and reduce vascular complications.Few studies have investigated diabetes self‐care behaviours and their associations with health literacy and self‐efficacy in people diagnosed with serious mental illness. What the paper adds to existing knowledge?: Diabetes self‐care behaviours in people diagnosed with serious mental illness were suboptimal; the least frequently performed self‐care activities were self‐monitoring of blood glucose.Factors associated with diabetes self‐care behaviours are gender, age, communicative and critical health literacy and self‐efficacy.Self‐efficacy is the strongest predictor of self‐care behaviours among people diagnosed with comorbid serious mental illness and type 2 diabetes. What are the implications of practice?: Mental health nurses should assess diabetes‐specific health literacy of people diagnosed with serious mental illness to ensure that they possess the knowledge and skills related to diabetes self‐care.When treating young people and those with newly diagnosed type 2 diabetes, nurses should incorporate strategies to minimise their perceptions of diabetes‐related distress and increase their confidence in managing comorbid diabetes. Introduction: People diagnosed with serious mental illness (SMI) experience greater challenges in managing their type 2 diabetes mellitus (T2DM) than do those diagnosed with T2DM alone. Aim: This study investigated diabetes self‐care activities and the factors associated with these activities in people diagnosed with SMI in a hospital setting. Methods: A cross‐sectional correlational study was conducted among 126 people diagnosed with comorbid SMI and T2DM in Taipei, Taiwan, between October 2020 and April 2021. Data were collected using self‐report questionnaires and a chart review. Three‐step hierarchical multiple regression analysis was used to identify factors associated with diabetes self‐care behaviours. Results: Diabetes self‐care behaviours in people diagnosed with SMI were suboptimal overall. Hierarchical multiple regression analyses revealed that age (β = 0.18, p =.037) and self‐efficacy (β = 0.27, p =.004) significantly associated with diabetes self‐care behaviours. Discussion: Self‐efficacy is the strongest predictor of self‐care behaviours among people diagnosed with comorbid SMI and T2DM. Implications for Practice: Mental health professionals should focus on enhancing confidence in managing comorbid diabetes in people diagnosed with comorbid SMI, especially young people and those with newly diagnosed T2DM. [ABSTRACT FROM AUTHOR]