[Show abstract][Hide abstract] ABSTRACT: In principle, the spin-½ plutonium-239 ((239)Pu) nucleus should be active in nuclear magnetic resonance spectroscopy. However, its signal has eluded detection for the past 50 years. Here, we report observation of a (239)Pu resonance from a solid sample of plutonium dioxide (PuO(2)) subjected to a wide scan of external magnetic field values (3 to 8 tesla) at a temperature of 4 kelvin. By mapping the external field dependence of the measured resonance frequency, we determined the nuclear gyromagnetic ratio (239)γ(n)(PuO(2))/2π to be 2.856 ± 0.001 megahertz per tesla (MHz/T). Assuming a free-ion value for the Pu(4+) hyperfine coupling constant, we estimated a bare (239)γ(n)/2π value of ~2.29 MHz/T, corresponding to a nuclear magnetic moment of μ(n) ≈ 0.15μ(N) (where μ(N) is the nuclear magneton).