Layer-by-layer self-assembly is an approach to develop an ultrathin film on solid support by alternate exposure to positive and negative species with spontaneous deposition of the oppositely charged ions. This paper summarizes various approaches used for fabrication of layer-by-layer self-assembly as well as their utility to produce various devices. The layer-by-layer technique is basically used for formation of multilayer films. A variety of nanomaterials use it for the modification of films to enhance their resultant durability as well as strength. Studies have shown that many different types of materials can be used for fabrication of multilayers. Recently the layer-by-layer self-assembly technique has also been used for fabrication of gas sensors, hydrogen sensors and solar-based cells. Various methods, such as spin deposition, calcinations, and dry-transfer printing are being used for fabrication of thin films. In this review, the author summarizes the various interesting properties as well as fabrication strategies of layer-by-layer self-assembly.