The magnetic field response of the transport properties of novel materials and then the large magnetoresistance effects are of broad importance in both science and application. We report large transverse magnetoreistance (the magnetoresistant ratio ~ 1.3 × 105% in 2 K and 9 T field, and 4.3 × 106% in 0.4 K and 32 T field, without saturation) and field-induced metal-semiconductor-like transition, in NbSb2 single crystal. Magnetoresistance is significantly suppressed but the metal-semiconductor-like transition persists when the current is along the ac-plane. The sign reversal of the Hall resistivity and Seebeck coefficient in the field, plus the electronic structure reveal the coexistence of a small number of holes with very high mobility and a large number of electrons with low mobility. The large MR is attributed to the change of the Fermi surface induced by the magnetic field which is related to the Dirac-like point, in addition to orbital MR expected for high mobility metals.