We study the nuclear magnetic relaxation rate and Knight shift in the presence of the orbital and quadrupole interactions for three-dimensional Dirac electron systems (e.g., bismuth-antimony alloys). By using recent results of the dynamic magnetic susceptibility and permittivity, we obtain rigorous results of the relaxation rates (1/T 1 ) orb and (1/T 1 ) Q , which are due to the orbital and quadrupole interactions, respectively, and show that (1/T 1 ) Q gives a negligible contribution compared with (1/T 1 ) orb . It is found that (1/T 1 ) orb exhibits anomalous dependences on temperature T and chemical potential µ. When µ is inside the band gap, (1/T 1 ) orb ∼ T 3 log(2T/ω 0 ) for temperatures above the band gap, where ω 0 is the nuclear Larmor frequency. When µ lies in the conduction or valence bands, (1/T 1 ) orb ∝ T k 2 F log(2|v F |k F /ω 0 ) for low temperatures, where k F and v F are the Fermi momentum and Fermi velocity, respectively. The Knight shift K orb due to the orbital interaction also shows anomalous dependences on T and µ. It is shown that K orb is negative and its magnitude significantly increases with decreasing temperature when µ is located in the band gap. Because the anomalous dependences in K orb is caused by the interband particle-hole excitations across the small band gap while (1/T 1 ) orb is governed by the intraband excitations, the Korringa relation does not hold in the Dirac electron systems.