Inadequate numbers, maldistribution, attrition, and inadequate skill‐mix are widespread health and care workforce (HCWF) challenges. Intersectoral—inclusive of different government sectors, non‐state actors, and the private sector—collaboration and action are foundational to the development of a responsive and sustainable HCWF. This review presents evidence on how to work across sectors to educate, recruit, and retain a sustainable HCWF, highlighting examples of the benefits and challenges of intersectoral collaboration. We carried out a scoping review of scientific and grey literature with inclusion criteria around intersectoral governance and mechanisms for the HCWF. A framework analysis to identify and collate factors linked to the education, recruitment, and retention of the HCWF was carried out. Fifty‐six documents were included. We identified a wide array of recommendations for intersectoral activity to support the education, recruitment, and retention of the HCWF. For HCWF education: formalise intersectoral decision‐making bodies; align HCWF education with population health needs; expand training capacity; engage and regulate private sector training; seek international training opportunities and support; and innovate in training by leveraging digital technologies. For HCWF recruitment: ensure there is intersectoral clarity and cooperation; ensure bilateral agreements are ethical; carry out data‐informed recruitment; and learn from COVID‐19 about mobilising the domestic workforce. For HCWF retention: innovate around available staff, especially where staff are scarce; improve working and employment conditions; and engage the private sector. Political will and commensurate investment must underscore any intersectoral collaboration for the HCWF.