The development of high-performance elastomers that are simultaneously

strong, crack-tolerant, and wear-resistant remains a persistent challenge.

Herein, we design bio-inspired semicarbazide chain extender featuring highdensity

hydrogen-bonding sites to synthesize poly(urethane-urea) (PUU). The

use of two such extenders creates geometric confinement that promotes

ordered H-bonding arrays, which synergistically enhances the mechanical

performance. The resulting PUU-HI elastomer exhibits a nanoscale-ordered

phase-separated structure and maximized H-bonding, achieving a tensile

strength of 120.2MPa, toughness of 400.5 MJ m?3 and true fracture stress of

1.3 GPa, even surpassing spider silk. The architecture additionally delivers high

crack tolerance, fatigue resistance, and high wear resistance, making it ideal

for stable, long-term used triboelectric nanogenerator interfaces. Solid-state

NMR reveals the geometric-confinement-induced ordered and high-density Hbonding

structure in hard domain for efficient energy dissipation. By designing

tailored H-bonding motifs and amplifying supramolecular interactions via

geometric confinement, this work offers a promising strategy for developing

mechanically robust and durable elastomers.