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Cellulose, the abundantly available natural biopolymer, has the potential to be a next generation wonder material. The motivation behind this thesis stems from the efforts to obtain mechanical properties of two novel cellulose-based materials, which were fabricated using top-down (densified engineered wood) and bottoms-up (graphite-cellulose composite) approaches. It was observed that the mechanical properties of both the engineered wood (strength~596 MPa; toughness ~3.9 MJ/m3) and cellulose-graphite composite (strength~715 MPa; toughness ~27.7 MJ/m3) surpassed the equivalent features of other conventional structural materials (e.g., stainless steel, Al alloys etc.). However, these appealing properties are still considerably inferior to individual cellulose fibrils whose diameters are in the order of nanometers. A significant research effort needs to be initiated to effectively transfer the mechanical properties of the hierarchical cellulose fibers from the atomistic level to the continuum. To achieve that, a detailed understanding of the interplay of cellulose molecular chains that affects the properties of the bulk cellulosic material, is needed. Modeling investigations can shed light on such underlying mechanisms that ultimately dictate multiple properties (e.g., mechanics, thermal transport) of these cellulosic materials.

To that end, this thesis (1) applies molecular dynamics simulations to decipher why microfibers made of aligned nanocellulose and carbon nanotubes possess excellent mechanical strength, along with understanding the role of water in fully recovering elastic wood under compression; (2) delineates an atomistically informed multi-scale, scalable, coarse grained (CG) modeling scheme to study the effect of cellulose fibers under different representative loads (shearing and opening), and to demonstrate a qualitative guideline for cellulose nanopaper design by understanding its failure mechanism; (3) utilizes the developed multi-scale CG scheme to illustrate the reason why a hybrid biodegradable straw, experimentally fabricated using both nano- and micro-fibers, exhibits higher mechanical strength than individual straws that were built using only nano or microfibers; (4) investigates the individual role of nanocellulose and boron nitride nanotubes in increasing the mechanical properties (tensile strength, stiffness) of the derived nanocellulose/boron-nitride nanotube hybrid material; (5) employs reverse molecular dynamics approach to explore how the boron nitride nanotube based fillers can improve thermal conductivity (k) of a nanocellulose derived material.

In addition, this thesis also intends to educate the readers on two perspectives. The common link connecting them is the method of engineering intermolecular bonds. The first discussion presents a few novel mechanical design strategies to fabricate high-performance, cellulose-based functional materials. All these strategies are categorized under a few broad themes (interface engineering, topology engineering, structural engineering etc.). Another discussion has been included by branching out to other materials that, like nanocellulose, can also be tuned by intermolecular bonds engineering to achieve unique applications. Avenues for future work have been suggested which, hopefully, can act as a knowledge base for future researchers and help them formulate their own research ideas. This thesis extends the fundamental knowledge of nanocellulose-based polymer sciences and aims to facilitate the design of sustainable and programmable nanomaterials.