Optimising the scale and deployment of community health workers (CHWs) is important for maximizing geographical accessibility of integrated primary health care (PHC) services. Yet little is known about approaches for doing so. We used geospatial analysis to model optimised scale-up and deployment of CHWs in Mali, to inform strategic and operational planning by the Ministry of Health and Social Development. Accessibility catchments were modelled based on travel time, accounting for barriers to movement. We compared geographic coverage of the estimated population, under-five deaths, and plasmodium falciparum (Pf) malaria cases across different hypothetical optimised CHW networks and identified surpluses and deficits of CHWs compared to the existing CHW network. A network of 15 843 CHW, if optimally deployed, would ensure that 77.3% of the population beyond 5 km of the CSCom (community health centre) and CSRef (referral health facility) network would be within a 30-minute walk of a CHW. The same network would cover an estimated 59.5% of U5 deaths and 58.5% of Pf malaria cases. As an intermediary step, an optimised network of 4 500 CHW, primarily filling deficits of CHW in the regions of Kayes, Koulikoro, Sikasso, and Ségou would ensure geographic coverage for 31.3% of the estimated population. There were no important differences in geographic coverage percentage when prioritizing CHW scale-up and deployment based on the estimated population, U5 deaths, or Pf malaria cases. Our geospatial analysis provides useful information to policymakers and planners in Mali for optimising the scale-up and deployment of CHW and, in turn, for maximizing the value-for-money of resources of investment in CHWs in the context of the country's health sector reform. Countries with similar interests in optimising the scale and deployment of their CHW workforce may look to Mali as an exemplar model from which to learn.