Nanocomposite hydrogels are prepared combining polymer brush-modified ‘hard’ cellulose nanocrystals (CNC) and ‘soft’ polymeric domains, and bound together by cucurbituril (CB) supramolecular crosslinks, which allow dynamic host–guest interactions as well as selective and simultaneous binding of two guests, i.e., methyl viologen (the first guest) and naphthyl units (the second guest). CNCs are mechanically strong colloidal rods with nanometer-scale lateral dimensions, which are functionalized by surface-initiated atom transfer radical polymerization to yield a dense set of methacrylate polymer brushes bearing naphthyl units. They can then be non-covalently cross-linked through simple addition of poly(vinyl alcohol) polymers containing pendant viologen units as well as CBs in aqueous media. The resulting supramolecular nanocomposite hydrogels combine three important criteria: high storage modulus (G′ > 10 kPa), rapid sol–gel transition (<6 s), and rapid self-healing even upon aging for several months, as driven by balanced colloidal reinforcement as well as the selectivity and dynamics of the CB three-component supramolecular interactions. Such a new combination of properties for stiff and self-healing hydrogel materials suggests new approaches for advanced dynamic materials from renewable sources.