A smart bilayer of AG@CNT/AG composed of carbon nanotubes (CNTs) and Agarose (AG) is developed. TiO2 pattern which partly reflects light is introduced at the bilayer surface, giving rise to a spatially-selective photothermal effect that can be used to induce shape-programmed motility. The TiO2 patterning can also modulate the bilayer for chiral motions through manipulating humidity.