This work describes chromatographic radionuclide generator systems for the production of actinides and natural decay series elements. The generator systems begin with alpha emitting parent radioisotopes with half-lives (T1/2) of greater than one year and produce alpha or beta emitting radioisotopes with half-lives of hours to days. Chromatographic systems were chosen to minimize radiolytic damage to chromatographic supports, preserve the parent activity for repeated use, provide high purity daughter radionuclide tracers, and to minimize or eliminate the need for evaporation of solutions of the parent or daughter nuclides. Useful secondary separations involving the daughters of the initial parent radionuclide are also described. Separation systems for 210Bi, 210Po, 211Pb, 212Pb, 223Ra, 224Ra, 225Ra, 225Ac, 227Th, 228Th, 231Th, 234Th, and 239Np are outlined in detail.