Hydrogels are biocompatible polymer networks; however, they have the disadvantage of having poor mechanical properties. Herein, the mechanical properties of host-guest hydrogels were increased by adding a filler and incorporating other noncovalent interactions. Cellulose was added as a filler to the hydrogels to afford a composite. Citric acid-modified cellulose (CAC) with many carboxyl groups was used instead of conventional cellulose. The preparation began with mixing an acrylamide-based alpha CD host polymer (p-alpha CD) and a dodecanoic acid guest polymer (p-AADA) to form supramolecular hydrogels (p-alpha CD/p-AADA). However, when CAC was directly added to p-alpha CD/p-AADA to form biocomposite hydrogels (p-alpha CD/p-AADA/CAC), it showed weaker mechanical properties than p-alpha CD/p-AADA itself. This was caused by the strong intramolecular hydrogen bonding (H-bonding) within the CAC, which prevented the CAC reinforcing p-alpha CD/p-AADA in p-alpha CD/p-AADA/CAC. Then, calcium chloride solution (CaCl2) was used to form calcium ion (Ca2+) complexes between the CAC and p-alpha CD/p-AADA. This approach successfully created supramolecular biocomposite hydrogels assisted by Ca2+ complexes (p-alpha CD/p-AADA/CAC/Ca2+) with improved mechanical properties relative to p-alpha CD/p-AADA hydrogels; the toughness was increased 6-fold, from 1 to 6 MJ/m(3). The mechanical properties were improved because of the disruption of the intramolecular H-bonding within the CAC by Ca2+ and subsequent complex formation between the carboxyl groups of CAC and p-AADA. This mechanism is a new approach for improving the mechanical properties of hydrogels that can be broadly applied as biomaterials.