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Superior strong and tough structural materials are highly desirable in engineering applications. However, it remains a big challenge to combine these two mutually exclusive mechanical properties into one body. In the work, an ultrastrong and tough cellulosic material was fabricated by a two-step process of delignification and water molecule-induced hydrogen bonding under compression. The strong and tough cellulosic material showed enhanced tensile strength (352 MPa vs. 56 MPa for natural wood) and toughness (4.1 MJ m⁻³ vs. 0.42 MJ m⁻³ for natural wood). The mechanical behaviors of ultrastrong and tough bulk material in a tensile state were simulated by finite element analysis (FEA) using mechanical parameters measured in the experiment. FEA results showed that the tensile strength and toughness gradually simultaneously improved with the increase in moisture content, demonstrating that water molecules played an active role in fabricating strong and tough materials, by plasticizing and forming hydrogen bonding among cellulose nanofibrils.