Optically addressable nanostructured capsules of polyelectrolyte multilayers containing gold nanoparticles are prepared via layer-by-layer colloid templating. The nanocomposite capsule shell, due to the presence of the metal nanoparticles, can be addressed with laser light in the near-infrared (NIR) to induce morphological changes in the capsules (see Figure). Enzyme encapsulated within these capsules is released remotely and on demand with nanosecond laser pulses in the NIR, while retaining its activity.