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Scalable, low-density and flexible aerogels offer a unique combination of excellent mechanical properties and scalable manufacturability. Herein, we report the fabrication of a family of low-density, ambient-dried and hydrophobic poly(isocyanurate–urethane) aerogels derived from a triisocyanate precursor. The bulk densities ranged from 0.28 to 0.37 g cm −3 with porosities above 70% v/v. The aerogels exhibit a highly stretchable behavior with a rapid increase in the Young's modulus with bulk density (slope of log–log plot > 6.0). In addition, the aerogels are very compressible (more than 80% compressive strain) with high shape recovery rate (more than 80% recovery in 30 s). Under tension even at high strains ( e.g. , more than 100% tensile strain), the aerogels at lower densities do not display a significant lateral contraction and have a Poisson's ratio of only 0.22. Under dynamic conditions, the properties ( e.g. , complex moduli and dynamic stress–strain curves) are highly frequency- and rate-dependent, particularly in the Hopkinson pressure bar experiment where in comparison with quasi-static compression results, the properties such as mechanical strength were three orders of magnitude stiffer. The attained outcome of this work supports a basis on the understanding of the fundamental mechanical behavior of a scalable organic aerogel with potential in engineering applications including damping, energy absorption, and substrates for flexible devices.