A layer-by-layer (LbL) assembly of alternating layers of oppositely charged polyelectrolytes and nanoparticles provides the formation of 5 –500 nm thick films with monolayers of various substances growing in a pre-set sequence on any substrates at a growth step of about 1 nm. This technique was called “molecular beaker epitaxy” meaning by this that with simple instruments (exploiting the materials self-assembly tendency) one can get molecularly organized films similar to the ones obtained with highly sophisticated and expensive molecular beam epitaxy technology for metals and semiconductors. LbL films can coat solid supports, slides, silicon wafers, plastics and fiber optics (2D nanoassembly). Besides, LbL films can be assembled on micro- and nanotemplates, such as 100-500 nm diameter latex, drug microcrystals, biological cells and even viruses, providing by this method for 3D nanoassembly. Polymeric nanoshells also can be prepared with LbL assembly.