AbstractData collected by the Fast Imaging Plasma Spectrometer (FIPS) aboard the MErcury Surface, Space ENvironment, GEochemistry, and Ranging (MESSENGER) spacecraft showed singly charged Na+‐group ions at energies of between 1 and 13 keV in Mercury's northern planetary cusp. Most of these ions are likely formed by either photoionization or charge exchange of exospheric Na atoms, with initial energies of approximately 1 eV or less. FIPS observations did not establish which acceleration mechanism most reasonably accounts for this energy gain. Using the Adaptive Mesh Particle Simulator (AMPS) model, we undertake kinetic simulations of 1 eV Na+ test particles through the electric and magnetic fields output from the Block Adaptive Tree Solar wind Roe‐type Upwind Scheme (BATSRUS) global magnetohydrodynamic (MHD) model of Mercury's magnetosphere, in search of plausible explanations for the source of this energization. We find that Na+ with initial energy of 1 eV are readily picked up by the Dungey cycle return flow in the dayside magnetosphere. In some cases, this flow provides the energy for the ions to escape into the magnetosheath, and in other cases it energizes the ions to hundreds of eV before they pass immediately into the cusp. Those that escape can be rapidly picked up into the magnetosheath flow, where they are accelerated by pickup again up to tens of keV. These one‐ and two‐stage pickup processes on Mercury's dayside can account for the energies of many of the Na+ ions observed in Mercury's northern magnetospheric cusp by MESSENGER.