Kundt spacetimes are of great importance to general relativity. We show that a Kundt spacetime is a Lorentz manifold with a non-singular isotropic geodesic vector field having its orthogonal distribution integrable and determining a totally geodesic foliation. We give the local structure of Kundt spacetimes and some properties of left invariant Kundt structures on Lie groups. Finally, we classify all left invariant Kundt structures on three-dimensional simply connected unimodular Lie groups.