A great number of stimuli-responsive materials have been reported in the recent years and they find applicability in fields ranging from optoelectronics, surface coatings, photonics and biomedicine. A particular attractive class of stimuli-responsive materials is comprised by photo-responsive materials as light is an environment-friendly stimulus and can be applied remotely, in a non-invasive manner. Photo-responsive materials have been the subject of many investigations over the past decade due to their potential applications, particularly in the design and development of memory devices, artificial muscles, soft-actuators and drug delivery, among others[1]. In the field of photo-responsive polymers, the layer-by-layer (LbL) approach offers a simple and effective method to fabricate uniform thin films capable of photo-modulation. In this context, we are focusing our investigations on the synthesis of LbL coatings based on new photochromic norbornenes polymers bearing spiropyran side groups. We have shown that these LbL coatings are capable of disassembling upon photostimulation. When used for the coating of microcapsules, these polymers have the ability to be used for photo-controlled drug delivery. [1] L. Florea, D. Diamond, F. Benito-Lopez, Macromol. Mater. Eng. 2012, 297, 1148.