Background Serious mental illness (SMI) — which comprises long-term conditions such as schizophrenia, bipolar disorder, and other psychoses — has enormous costs for patients and society. In many countries, people with SMI are treated solely in primary care, and have particular needs for physical care. Aim The objective of this study was to systematically review the literature to create a list of quality indicators relevant to patients with SMI that could be captured using routine data, and which could be used to monitor or incentivise better-quality primary care. Design and setting A systematic literature review, combined with a search of quality indicator databases and guidelines. Method The authors assessed whether indicators could be measured from routine data and the quality of the evidence. Results Out of 1847 papers and quality indicator databases identified, 27 were included, from which 59 quality indicators were identified, covering six domains. Of the 59 indicators, 52 could be assessed using routine data. The evidence base underpinning these indicators was relatively weak, and was primarily based on expert opinion rather than trial evidence. Conclusion With appropriate adaptation for different contexts, and in line with the relative responsibilities of primary and secondary care, use of the quality indicators has the potential to improve care and to improve the physical and mental health of people with SMI. However, before the indicators can be used to monitor or incentivise primary care quality, more robust links need to be established, with improved patient outcomes.