The superconducting phase diagram for a quasi-two-dimensional organic superconductor, κ-(BEDT-TTF)2Cu[N(CN)2]Br, was studied using pulsed magnetic field penetration depth measurements under rotating magnetic fields. At low temperatures, Hc2 was abruptly suppressed even by small tilts of the applied fields owing to the orbital pair-breaking effect. In magnetic fields parallel to the conducting plane, the temperature dependence of the upper critical field Hc2 exhibited an upturn and exceeded the Pauli limit field HP in the lower temperature region. Further analyses with the second derivative of the penetration depth showed an anomaly at 31–32 T, which roughly corresponded to HP. The origin of the anomaly should not be related to the orbital effect, but the paramagnetic effect, which is almost isotropic in organic salts, because it barely depends on the field angle. Based on these results, the observed anomaly is most likely due to the transition between the Bardeen-Cooper-Schrieffer (BCS) and the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) states. Additionally, we discuss the phase diagram and physical parameters of the transition by comparing them with other FFLO candidates.