Utilization of reversible interactions as sacrificial bonds in biopolymers is critical for the integral synthesis of mechanically superior biological materials. In this work, cellulose nanofibrils (CNFs) reinforced covalent polyacrylamide (PAAm) composite hydrogels are immersed into multivalent cation (Ca2+, Zn2+, Al2+, and Ce3+) aqueous solution to form ionic association among CNFs, leading to the ionic covalent cross-linke dhydrogels. The cations promote the formation of porous networks of nanofibrils by screening the repulsive negative charges on CNF surface and dominate the mechanical properties and self-recovery efficiency of the hydrogels, resulting in mechanically reinforced ionic hydrogels with stiff (Young's modulus 257 kPa) and tough properties (fracture toughness 386 kJ/m(3)). The in situ Raman spectroscopy during stretching corroborates the stress transfer medium of CNF, and the microscopic morphologies of stable crack propagation validates that the multiple toughening mechanisms occur in a balanced energy dissipation manner, enabling synergistic combination of stiffness and toughness. Moreover, the depth-sensing instrumentation by indentation test also demonstrates that the CNF ionic coordination contributes simultaneous improvement in hardness and elasticity by as much as 600% compared to those pristine gels. This work demonstrates a facile way to transfer nanoscale building blocks to bulk elastomers with tunable dynamic properties and may provide a new prospect for the rational design of CNF reinforced hydrogels for applications where high-bearing capability is needed.