Nanoarchitectonics approaches can produce functional materials from tiny units through combination of various processes including atom/molecular manipulation, chemical conversion, self-assembly/self-organization, microfabrication, and bio-inspired procedures. Existing fabrication approaches can be regarded as fitting into the same concept. In particular, the so-called layer-by-layer (LbL) assembly method has huge potential for preparing applicable materials with a great variety of assembling mechanisms. LbL assembly is a multistep process where different components can be organized in planned sequences while simple alignment options provide access to superstructures, for example helical structures, and anisotropies which are important aspects of nanoarchitectonics. In this article, newly-featured examples are extracted from the literature on LbL assembly discussing trends for composite functional materials according to (i) principles and techniques, (ii) composite materials, and (iii) applications. We present our opinion on the present trends, and the prospects of LbL assembly. While this method has already reached a certain maturity, there is still plenty of room for expanding its usefulness for the fabrication of nanoarchitectonics-based materials and devices.