For creation of autonomous microrobots which are able to move under conditions of a constant environment and a constant energy supply, a mechanism for maintenance of mechanical motion with a capacity for self-control is required. This requirement, known as self-organisation, represents the ability of a system to evade equilibrium through formation of a spatio-temporal pattern. Following our previous finding of a self-oscillatory flipping motion of an azobenzene-containing co-crystal, we present here regulation of the flipping motion by a light-receiving sensor molecule in relation to the alignment and role of azobenzene molecules in crystals. In the anisotropic structure, a specific azobenzene molecule acts as a reaction centre for the conversion of light to a mechanical function process, while the other molecules act as modulators for spatio-pattern regulation. The present results demonstrate that autonomously drivable molecular materials can exhibit information-responsive, self-sustainable motion by incorporating stimulus-responsive sensors.