Utilization of unique properties of nanoscale graphene in macroscale materials requires a thoughtful selection of processing method(s). Here we review different materials assembly techniques which result in layered composite reminiscent of many biomaterials with the focus on layer-by-layer (LBL) assembly, vacuum-assisted flocculation (VAF), and others. Critical evaluation of LBL and its comparison to other solution-based methods of materials assembly using the abundant experimental data with graphene and graphene oxide is the main essence of this review. We compare several fundamental characteristics and applications being discussed for graphene-based material such as transparent conducting films, field effect transistors, lithium ion batteries, supercapacitors, solar cells, sensors and polymer nanocomposites, highlighting the strengths, the weaknesses, and expected points of further developments of different techniques. The principle goal to be achieved in the future is to define much better effective implementation of layer-by-layer assembly and other techniques resulting in layered composites taking into account potential technological areas of applications.

This paper was originally published in Nano Today (2012) 7, 430-447.

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