Recently, certain challenges and accompanying drawbacks have emerged in the preparation of high-strength and tough polymer hydrogels. Insights from wood science highlight the role of the intertwined molecular structure of lignin and crystalline cellulose in contributing to wood's strength. Herein, we immersed prestretched poly(vinyl alcohol) (PVA) polymer hydrogels into a solution of nanosized lignosulfonate sodium (LS), a water-soluble anionic polyelectrolyte, to creatively reconstruct this similar structure at the molecular scale in hydrogels. The nanosized LS effectively fixed and bundled the prestretched PVA polymers while inducing the formation of dense crystalline domains within the polymer matrix. Consequently, the interwoven structure of crystalline PVA and LS conferred good strength to the composite hydrogels, exhibiting a tensile strength of up to ∼23 MPa, a fracture strain of ∼350%, Young's modulus of ∼17 MPa, toughness of ∼47 MJ/m