For the hexagonal ferromagnet UNi2, an unusual 5fform factor for uranium has been observed, indicating a large orbital contribution to the total moment. We report on self‐consistent electronic structure calculations for the hexagonal Laves phase (C14) compound UNi2, taking both spin and orbital contributions to the total moment into account. In a constrained calculation, where the spin moment is chosen to agree with experiment, very good agreement with the experimental form factor is obtained. In the analysis of the form factor both the 6dand the 5felectrons are taken into account giving improved agreement with experiment.