In this work, we investigate a novel approach to prepare high-performance alpha-particle solid sources fabricated on diamond thin support layers, offering the properties of diamond such as a low-Z material with corrosion and mechanical hardness. As-prepared solid sources onto boron-doped-diamond (BDD) substrate exhibited high performance of the autoradiography and spectroscopic resolution at the level of other more conventional materials such as stainless steel. A straightforward precipitation process in the Na2SO4 or NaNO3 simple electrolytes under mild experimental conditions with a low current of several mA.cm−2 were successfully developed onto BDD substrates for deposition of single 241Am as well as 239Pu, 241Am, and 244Cm mixed radionuclides. The results demonstrate that solid sources deposited onto such BDD substrates can match the performance of those prepared onto stainless steel substrates with excellent uniformity and high-resolution spectroscopy, together combining the robustness, chemical resilience, and X-ray transparence of the diamond. Alpha-particle spectra exhibiting a low full width at half maximum (FWHM) of 12.5 keV at the energy of 5.485 MeV (241Am) could be practically obtained for BDD substrates.