The optimum conditions were investigated for the production of 61Cu by the alpha-particle bombardment of natural nickel. Formation cross-sections and thick-target yields were obtained for most of the reaction products in the energy range from 10 to 40 MeV. When the incident alpha energy of 21 MeV was chosen, after 2 hr of cooling 2.1 mCi/μA·hr of 61Cu could be produced with a 60Cu contamination of less than 1%. The other reaction products were also analyzed in terms of the corresponding nuclear reactions, and excitation functions were deduced for the 58Ni and 60Ni target nuclides.