Super-compressible foam-like carbon nanotube films [1][2][3][4][5][6][7] have been reported to exhibit highly nonlinear viscoelastic behavior in compression similar to soft tissue. [4] Their unique combination of light weight and exceptional electrical, thermal, and mechanical properties have helped identify them as viable building blocks for more complex nanosystems and as stand-alone structures for a variety of different applications. In the as-grown state, their mechanical performance is limited by the weak adhesion between the tubes, controlled by van der Waals forces, and the substrate allowing the forests to split easily and to have low resistance in shear.[5] Under axial compression loading carbon nanotubes have demonstrated bending, buckling, [8] and fracture [9] (or a combination of the above) depending on the loading conditions and the number of loading cycles. [4] In this work, we study the strain rate effects on the mechanical properties of carbon nanotube forests and report several related interesting new phenomena. We partially anchor [10] dense vertically aligned foam-like forests of carbon nanotubes on a thin, flexible polymer layer to provide structural stability, particularly at the higher strain rates. The goal of the anchoring was also to create versatile nanosystems, which integrate the excellent nanotube properties in a light-weight portable system. We test the sample under quasi-static indentation loading and under impact loading and report a variable nonlinear response and different elastic recoveries with varying strain rates. A Bauschinger-like effect is observed at very low strain rates while buckling and the formation of permanent defects in the tube structure is reported at very high strain rates. Using high-resolution transmission microscopy we observe for the first time the delamination and crumbling of carbon nanotube walls. These polymer-anchored CNT foams are reported to behave as conductive nanostructured layers, suitable as fundamental building blocks for a variety of different applications, or as new self-standing application-ready materials with potential employment as actuators, impact absorbers, or as layered components for the creation of acoustic dampers.Because of the excellent thermal, electronic and mechanical properties, vertically aligned carbon nanotube (CNT) arrays have been proposed for several potential applications, ranging from biomimetic adhesives similar to spider's and gecko's feet, [11] to nanobrushes, [12] vibration damping layers, [6] and multifunctional composites, [13] but their development into successful commercial applications has been limited by their weak adhesion to the growth substrate, resulting in poor resistance to shear. In the present work we grew long, vertically-aligned multiwall CNTs (Fig. 1a), transferred and anchored them in thin polymer layers (Fig. 1b), and tested their mechanical response. While the nanotubes appear to be vertically aligned throughout the entire thickness of the sample (Fig. 1b), scanning electron microscopy (SEM) im...