Graphene
oxide liquid crystals (GOLCs) were exfoliated in a wide
variety of solvents (water, ethylene glycol (EG), N-methyl-2-pyrrolidone (NMP), and dimethylformamide (DMF)) by high-speed
shearing of graphite oxide. Quantitative polarized light imaging of
the equilibrium nematic phases of the lyotropic GOLCs gives insights
into the extent of aggregation and quantifiable textural features
such as domain size, d. Large nematic domains >100
μm with a high overall degree of order were obtained in water
and ethylene glycol, in contrast to ∼5–50 μm domains
in NMP and DMF at comparable volume fractions. Comprehensive rheological
studies of these GOLCs indicate that larger domains correlate with
higher viscosity and higher elasticity, and scaling analysis shows
a power-law dependence of the Ericksen number (Er) with domain size
(Er ∝ d
3.09). The improved understanding
of the relationship between the microstructure and flow properties
of GOLCs leads us to an approach of mixed solvent-based GOLCs as a
means to tune viscoelastic properties. We demonstrate this approach
for the formation of shear-aligned GOLC films for advanced flexible
electronic applications such as all-carbon conductive films and thermal
heaters.