Noncovalent cross-linked hydrogels with promising mechanical properties are on demand for applications in tissue engineering, flexible electronics, and actuators. However, integrating excellent mechanical properties with facile preparation for the design of hydrogen bond cross-linked hydrogels is still challenging. In this work, an advanced hydrogel was prepared from acrylamide and N-acryloyl phenylalanine by one-pot free-radical copolymerization. Owing to hydrophobicity-assisted multiple hydrogen bonding interactions among phenylalanine derivatives, the hydrogels exhibited fascinating mechanical behaviors: tensile strength of 0.35 MPa, elongation at break of 2100%, tearing energy of 1134 J/m2, and compression strength of 3.56 MPa. The hydrogels also showed robust elasticity and fatigue resistance, and the compression strength did not show any decline, even after 100 successive cycles, as well as promising self-recovery property. In addition, the cytotoxicity test in vitro proved that the hydrogel showed good biocompatibility with normal human liver cells (LO2 cells). The excellent stretchability, robust elasticity, high toughness, fatigue resistance, and biocompatibility of the hydrogel demonstrated its vast potential in the biomedical field and flexible electronic devices.