Dynamical simulations of the coupled rotational and orbital dynamics of binary near-Earth asteroid 66391 (1999 KW4) suggest that it is excited as a result of perturbations from the Sun during perihelion passages. Excitation of the mutual orbit will stimulate complex fluctuations in the orbit and rotation of both components, inducing the attitude of the smaller component to have large variation within some orbits and to hardly vary within others. The primary's proximity to its rotational stability limit suggests an origin from spin-up and disruption of a loosely bound precursor within the past million years.