Graphene-based sheets have stimulated great interest in many scientific disciplines and shown promise for wide potential applications. Among various ways of creating single atomic layer carbon sheets, a promising route for bulk production is to first chemically exfoliate graphite powders to graphene oxide (GO) sheets, followed by reduction to form chemically modified graphene (CMG). Due to the strong van der Waals attraction between graphene sheets, CMG tends to aggregate. The restacking of sheets is largely uncontrollable and irreversible, thus it reduces their processability and compromises properties such as accessible surface area. Strategies based on colloidal chemistry have been applied to keep CMG dispersed in solvents by introducing electrostatic repulsion to overcome the van der Waals attraction or adding spacers to increase the inter-sheet spacing. In this dissertation, two very different ideas that can prevent CMG aggregation without extensively modifying the material or introducing foreign spacer materials are introduced.

The van der Waals potential decreases with reduced overlapping area between sheets. For CMG, reducing the lateral dimension from micrometer to nanometer scale should greatly enhance their colloidal stability with additional advantages of increased charge density and decreased probability to interact. The enhanced colloidal stability of GO and CMG nanocolloids makes them especially promising for spectroscopy based bio-sensing applications.

For potential applications in a compact bulk solid form, the sheets were converted into paper-ball like structure using capillary compression in evaporating aerosol droplets. The crumpled graphene balls are stabilized by locally folded π-π stacked ridges, and do not unfold or collapse during common processing steps. They can tightly pack without greatly reducing the surface area. This form of graphene leads to scalable performance in energy storage. For example, planer sheets tend to aggregate and lose surface area. So their capacitive performance tends to decrease with increased loading level. But the crumpled balls can resist aggregation and retain high capacitance at high loading level. The crumpled graphene balls can be also used as expandable shells for wrapping lithium ion battery anode materials such as Si nanoparticles, which can accommodate their expansion/contraction without facture, and thus greatly improve the coulombic efficiency of the anode.