It is currently thought that the laser cooling of an ordered ion array, an ion crystal, is qualitatively the same as that of a single ion. We show that this assumption is strongly violated in recent experiments in Paul traps, due to ion micromotion. Our analysis demonstrates an unexpected laser damping instability that induces an ion-crystal order-chaos transition and also explains why ion crystals in Paul traps have been limited to less than 100 ions. We directly observe the effects of ion micromotion on the laser cooling of a single trapped Ba+ ion by a new technique. © 1989 The American Physical Society.