Theoretical predictions were made using TALYS-1.95(G) and EMPIRE 3.2 reaction-model codes for 69Ge, 67Ge, and medically used 68Ge, 67Ga, 68Ga, 65Zn, 64Cu radionuclides produced in the interaction of α-projectile with 66Zn-target at 10–40 MeV α-energies. Pearson’s statistical coefficients showed moderate to strong positive correlations between the theoretically predicted and experimentally measured production cross sections for radionuclides with practical medical applications. Furthermore, the present results indicated that a medium-sized cyclotron and a single α + 66Zn system (projectile + target system) might be an option for optimized production of 68Ge, 68Ga, 67Ga, 65Zn, and 64Cu radionuclides.