Owing　to　high　water　content　and　homogeneous　texture,　conventional　hydrogels　hardly　reach　satisfactory　mechanical　performance.　Tensile-resistant　groups　and　structural　heterogeneity　are　employed　to　fabricate　tough　hydrogels.　However,　those　techniques　significantly　increase　the　complexity　and　cost　of　material　synthesis,　and　have　only　limited　applicability.　Here,　it　is　shown　that　ultra-tough　hydrogels　can　be　obtained　via　a　unique　hierarchical　architecture　composed　of　chemically　coupled　self-assembly　units.　The　associative　energy　dissipation　among　them　may　be　rationally　engineered　to　yield　libraries　of　tough　gels　with　self-healing　capability.　Tunable　tensile　strength,　fracture　strain,　and　toughness　of　up　to　19.6　MPa,　20　000%,　and　135.7　MJ　cm　⁻(3)　are　achieved,　all　of　which　exceed　the　best　known　records.　The　results　demonstrate　a　universal　strategy　to　prepare　desired　ultra-tough　hydrogels　in　predictable　and　controllable　manners.