Nanocelluloses, both cellulose nanofibrils and cellulose nanocrystals, are gaining research traction due to their viability as key components in commercial applications and industrial processes. Significant efforts have been made to understand both the potential of assembling nanocelluloses, and the limits and prospectives of the resulting structures. This Review focuses on bottom-up techniques used to prepare nanocellulose-only structures, and details the intermolecular and surface forces driving their assembly. Additionally, the interactions that contribute to their structural integrity are discussed along with alternate pathways and suggestions for improved properties. Six categories of nanocellulose structures are presented: (1) powders, beads, and droplets; (2) capsules; (3) continuous fibres; (4) films; (5) hydrogels; and (6) aerogels and dried foams. Although research on nanocellulose assembly often focuses on fundamental science, this Review also provides insight on the potential utilization of such structures in a wide array of applications.