We report mechanical behavior and strain rate dependence of recoverability and energy dissipation in vertically aligned carbon nanotube (VACNT) bundles subjected to quasi-static uniaxial compression. We observe three distinct regimes in their stress–strain curves for all explored strain rates from 4 × 10^(–2) down to 4 × 10^(–4) /sec: (1) a short initial elastic section followed by (2) a sloped plateau with characteristic wavy features corresponding to buckle formation and (3) densification characterized by rapid stress increase. Load–unload cycles reveal a stiffer response and virtually 100% recoverability at faster strain rates of 0.04/sec, while the response is more compliant at slower rates, characterized by permanent localized buckling and significantly reduced recoverability. We propose that it is the kinetics of attractive adhesive interactions between the individual carbon nanotubes within the VACNT matrix that governs morphology evolution and ensuing recoverability. In addition, we report a 6-fold increase in elastic modulus and gradual decrease in recoverability (down to 50%) when VACNT bundles are unloaded from postdensification stage as compared with predensification. Finally, we demonstrate energy dissipation capability, as revealed by hysteresis in load–unload cycles. These findings, together with high thermal and electrical conductivities, position VACNTs in the “unattained-as-of-to-date-space” in the material property landscape
