Nanocellulose has emerged as a widely utilized building block in nanostructured materials due to its availability, sustainability, large surface area, and high stiffness and aspect ratio. The wet or dry elastoplastic properties of these materials are determined by the fibrils' stiffness, chemical properties, hemicellulose content, and the number of fibril contacts. However, the specific contributions and relative importance of each factor remain unclear. Therefore, this work was devoted to systematically comparing the material properties of gels, aerogels, and wet and dry sheets prepared from CNFs with different aspect ratios, chemical functionality, and hemicellulose content. The fibrils were prepared by chemical and mechanical processing of different pulps. By preserving the native structure as much as possible, higher aspect ratio fibrils can be obtained, which allows for the development of more mechanically robust materials. The results demonstrate that higher aspect ratios lead to more interconnected networks at a lower solids concentration, resulting in a more evenly distributed stress and longer-range stress transfer, yielding stiffer and more ductile materials. The most important finding was that the aspect ratio influences the network formation, resulting in different network topologies. The results were also compared to earlier published data and integrated into a theoretical beam-bending model for a complete elastoplastic description of the network properties, including the influence of fibril aspect ratio and chemical functionality. This information improves our understanding and description of nanofibril networks for which general models have been missing. It can be used to optimize nanofibril preparation and, hence, the resulting eco-friendly materials.