The spin of neodymium-141 was measured by the method of atomic beams and found to be 3/2. A lower limit placed on the hyperfine separation of the states with total angular momentum [formula] by second-order perturbation theory shows [formula]. A prerequisite for the determination of the nuclear spin from hyperfine-structure measurements is the knowledge of the electronic structure. The ground-state configuration of neodymium is known and the value is used throughout this work.