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.