This paper describes the generation of optimal atmospheric measurement networks for determining carbon dioxide fluxes over Australia using inverse methods. A Lagrangian particle dispersion model is used in reverse mode together with a Bayesian inverse modelling framework to calculate the relationship between weekly surface fluxes, comprising contributions from the biosphere and fossil fuel combustion, and hourly concentration observations for the Australian continent. Meteorological driving fields are provided by the regional version of the Australian Community Climate and Earth System Simulator (ACCESS) at 12 km resolution at an hourly timescale. Prior uncertainties are derived on a weekly timescale for biosphere fluxes and fossil fuel emissions from high-resolution model runs using the Community Atmosphere Biosphere Land Exchange (CABLE) model and the Fossil Fuel Data Assimilation System (FFDAS) respectively. The influence from outside the modelled domain is investigated, but proves to be negligible for the network design. Existing ground-based measurement stations in Australia are assessed in terms of their ability to constrain local flux estimates from the land. We find that the six stations that are currently operational are already able to reduce the uncertainties on surface flux estimates by about 30 %. A candidate list of 59 stations is generated based on logistic constraints and an incremental optimisation scheme is used to extend the network of existing stations. In order to achieve an uncertainty reduction of about 50 %, we need to double the number of measurement stations in Australia. Assuming equal data uncertainties for all sites, new stations would be mainly located in the northern and eastern part of the continent.