Graphene oxide (GO) is a near-2D material derived via oxidation of graphite and exploited in nanocomposites and optoelectronics. Following a literature review, the modified Tour-Dimiev (MTD) method was singled out for making GO, with the introduction of modifications tailored towards producing large sheets by starting with a large graphite size, tuning the oxidation conditions, employing temperature control and a modified wash routine. The product was characterized using wide-angle x-ray diffraction, x-ray photoelectron and Raman spectroscopy, revealing near completeness of graphite conversion, high oxygen content of GO and a comparable degree of defects to literature reports on the same. We imaged MTD-GO via fluorescence quenching microscopy (FQM) and atomic force microscopy (AFM). We compared the analytical capabilities of the image analysis software ImageJ with MATLAB, introducing several MATLAB subroutines to mitigate image analysis issues. We image-analyzed MTD-GO, concluding that GO size and thickness are statistically uncorrelated and described by lognormal and normal distributions respectively. We demonstrated that AFM captures small particles better than FQM, and that these two techniques can be combined to obtain a complete picture of polydisperse sample size distributions. Next, we modeled polydisperse dilute dispersions of oblate spheroids and discs in shear, uniaxial and biaxial extension using microhydrodynamic models found in the literature. We used the shear model to fit experimental shear data on a number of serially diluted sheet dispersions to obtain the dimensions and distributions thereof. The systems analyzed were MTD-GO, commercial GO before and after sonication, and a literature dataset on aqueous layered double hydroxides. Finally, we conducted novel Langmuir trough experiments with MTD-GO to understand the mechanisms surrounding the air-water interfacial assembly of GO. We were able to successfully transfer our films from the air-water interface onto a simple and versatile substrate such as surface-treated glass. We correlated film morphology in situ using Brewster Angle Microscopy and ex situ through FQM imaging of Langmuir-Blodgett-coated glass slides, to the pressure-area isotherm. We established that film packing occurs at low surface pressures. Finally, we showed that GO shows weak, pH-dependent intrinsic surface activity.