The low mechanical properties of high-water-content hydrogels often hinder their broad use in biomedical applications, especially in replacing/treating load-bearing tissues. Inspired by the protein structure of load-bearing tissues, we developed high-water-content hydrogels with excellent mechanical properties using a hydrophobic–hydrophilic copolymer strategy employing a benzene-based amphiphilic monomer, 5-acrylamidoisophthalic acid (AAI), as the major hydrophobic component and acrylamide (AAm) as the major hydrophilic component. The AAI monomer, connected with two –COOH functional groups, allowed the hydrogel to absorb excess water via H-bonding without compromising its homogeneity and structure. The AAI-rich hard-phase regions (via benzene–benzene interactions and hydrophobic associations) and AAm-rich soft-phase regions resulted in the high-water-content (∼80 wt%) hydrogel exhibiting a combination of good mechanical properties.