The central goal of this project is to establish a paradigm shift in material design by combining theory, modeling, and experimentation in a multiscale and synergistic manner to maximize the strength and toughness of nanocomposite materials that emulate the performance of natural nacre using graphene oxide. It is expected that graphene oxide sheets with optimal overlap geometry, bonded together by tunable chemistry, will mimic nacre. Specifically, this research will lead to characterization of the deformation mechanisms of multilayer nanocomposite systems through studies of the strength and stiffness of both the individual atomically thin sheets as well as their crosslinking elements. This project aims to develop a fundamental understanding of the roles that van der Waals interactions, hydrogen bonds, and chemical crosslinking, conformation, and geometrical assembly play in modulating the mechanical behavior of nanocomposite materials based on graphene oxide. The mechanical performance of functionalized graphene sheets and macroscopic oxidized-graphene materials will be optimized through a series of iterative synthesis-assembly-modeling cycles.