By virtue of the fact that its low-lying 2 ⌸ 3/2 state is paramagnetic, nitric oxide ͑NO͒ can be an effective agent for inducing nuclear spin relaxation during isolated binary collisions with other species. At the same time, the strong coupling between the electronic angular momentum and the internuclear axis of this particular molecule leads to a situation in which its effective magnetic moment depends critically on molecular motions that take place on the time scale of the collision. Here we present the results of an investigation in which the NMR-detected longitudinal nuclear relaxation rate T 1 −1 of room temperature 3 He gas adulterated with NO was measured as a function of NO density ͓͑NO͔͒ in two different magnetic fields. We find T 1 −1 = 0.0502͑3͒ ϫ͓NO͔ s −1 at 1.50 T, and T 1 −1 = 0.0506͑3͓͒NO͔ s −1 at 2.35 T, where ͓NO͔ is expressed in amagat. Under these conditions approximately two-thirds of the NO molecules occupy the diamagnetic 2 ⌸ 1/2 ground state and one-third occupy the paramagnetic 2 ⌸ 3/2 state. Our data can be understood in terms of a semiclassical treatment of collision dynamics that involves the paramagnetic moment autocorrelation function.