Indirect spin-spin interactions between nuclei bound in a molecule are well-known in nuclear magnetic resonance, but such interactions between unbound atoms are less well studied and are often assumed to be zero. We present the first precision calculation of this interaction between 129Xe and 3He nuclei in a gas. Relativistic, state-of-the-art electronic structure theory is used to compute the scalar coupling constant J(R) and the interatomic potential energy function, V(R), as functions of the Xe-He internuclear distance R. Using virial expansion we find the nuclear spin enhancement factor kappa = -0.0105 +/- 0.0015 in excellent agreement with recent experiments. This interaction is particularly important for precision measurements using nuclear spin co-magnetometers.