The 64Cu and 61Co radionuclides were produced simultaneously by irradiation of enriched 64Ni on a low energy proton-only cyclotron. Nickel targets were prepared by electrodeposition of enriched 64Ni (>95%) on Au backing at thicknesses of 25–225 mg/cm 2 with efficiencies >99%. Irradiations up to 30 μA for 8 h were performed with 11.4 MeV protons using a water-cooled target mounting. Radiochemical separation of 64Cu and 61Co from 64Ni was performed by chromatography of the chlorocomplexes in a single step using an anion exchange resin column with a yield >95%. Using this method, the Ni target material was recovered and re-plated for subsequent production runs with an overall efficiency >96%. The excitation function for the 64Ni(p,n) 64Cu reaction was measured and compared with published values. Experimental thick target saturation yields of 159 mCi/μA for 64Cu and 715 μCi/μA for 61Co were achieved. Typical specific activities of 64Cu were found to be 18.8±3.3 Ci/μmol.