We define Cayley structures as a field of Cayley’s ruled cubic surfaces over a four dimensional manifold and motivate their study by showing their similarity to indefinite conformal structures and their link to differential equations and the theory of integrable systems. In particular, for Cayley structures an extension of certain notions defined for indefinite conformal structures in dimension four are introduced, e.g., half-flatness, existence of a null foliation, ultra-half-flatness, an associated pair of second order ODEs, and a dispersionless Lax pair. After solving the equivalence problem we obtain the fundamental invariants, find the local generality of several classes of Cayley structures and give examples.