A new approach for the optimized design of high-homogeneity coil systems of the type used in nuclear magnetic resonance (NMR) applications is presented here. The approach effectively minimizes parameters such as the coil size in a solenoid magnet, or maximizes the gap/pole diameter ratio in a vertical gap NMR magnet, while preserving uniformity in an exceptionally large volume, resulting in novel coil geometries that have never been tried before. The approach can be applied to cylindrically symmetric coil systems with or without an active shield, as well as to long magnets of the type used in particle accelerators. Several practical examples are presented.