Naturally
derived cellulose nanocrystals (CNCs) and cellulose nanofibrils
(CNFs) are emerging nanomaterials that display high strength, high
surface area, and tunable surface chemistry, allowing for controlled
interactions with polymers, nanoparticles, small molecules, and biological
materials. Industrial production of nanocelluloses is increasing rapidly
with several companies already producing on the tons-per-day scale,
intensifying the quest for viable products across many sectors. While
the hydrophilicity of the nanocellulose interface has posed a challenge
to the use of CNCs and CNFs as reinforcing agents in conventional
plastics, it is a significant benefit for creating reinforced or structured
hydrogel composites (or, when dried, aerogels) exhibiting both mechanical
reinforcement and a host of other desirable properties. In this context,
this Review describes the quickly growing field of hydrogels and aerogels
incorporating nanocelluloses; over 200 references are summarized in
comprehensive tables covering the chemistry, preparation, properties,
and applications of “nanocellulose-only” and “nanocellulose-containing”
gels. Physical and chemical cross-linking strategies, postmodification
steps, and routes to control gel structure are discussed, along with
key developments and ongoing challenges in the field. Nanocellulose
hydrogels and aerogels show great promise in a wide range of biomedical,
energy storage, construction, separations, cosmetic, and food applications.