Two lowest-energy odd-parity atomic levels of actinium, 7s 2 7p 2 P o 1/2 , 7s 2 7p 2 P o 3/2 , were observed via two-step resonant laser-ionization spectroscopy and their respective energies were measured to be 7477.36(4) cm −1 and 12 276.59(2) cm −1 . The lifetimes of these states were determined as 668(11) ns and 255(7) ns, respectively. In addition, these properties were calculated using a hybrid approach that combines configuration interaction and coupled-cluster methods in good agreement. The data are of relevance for understanding the complex atomic spectra of actinides and for developing efficient laser-cooling and ionization schemes for actinium, with possible applications for high-purity medicalisotope production and future fundamental physics experiments with this atom.