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Natural materials such as bone and tooth achieve precisely tuned mechanical and interfacial properties by varying the concentration and orientation of their nanoscale constituents. However, the realization of such control in engineered foams is limited by manufacturing-driven tradeoffs among the size, order, and dispersion uniformity of the building blocks. It is demonstrated how to manufacture nanocomposite foams with precisely controllable mechanical properties via aligned carbon nanotube (CNT) growth followed by atomic layer deposition (ALD). By starting with a low density CNT forest and varying the ALD coating thickness, we realize predictable ≈1000-fold control of Young's modulus (14 MPa to 20 GPa, where E ∼ ρ 2.8), ultimate compressive strength (0.8 MPa to 0.16 GPa), and energy absorption (0.4 to 400 J cm–3). Owing to the continuous, long CNTs within the ceramic nanocomposite, the compressive strength and toughness of the new material are 10-fold greater than commercially available aluminum foam over the same density range. Moreover, the compressive stiffness and strength equal that of compact bone at 10% lower density. Along with emerging technologies for scalable patterning and roll-to-roll manufacturing and lamination of CNT films, coated CNT foams may be especially suited to multifunctional applications such as catalysis, filtration, and thermal protection.

Spatial mapping of strain fields within compressed carbon nanotube (CNT) array columns is achieved using digital image correlation (DIC) analysis of in situ scanning electron microscopy (SEM) image sequences. Full-field displacement and strain maps are generated based upon the motion of the constituent CNTs, which serve as a traceable high-contrast speckle pattern for DIC analysis. The deformation modes and CNT array buckling characteristics vary systematically as a function of column aspect ratio, including bending, crushing, and bottom-up buckle accumulation behaviors. In spite of disparate appearing deformation modes, strain maps indicate that CNT array buckling consistently initiates at 5% local principal strain (ϵ2) for all columns. The ability to quantitatively assess the deformation modes and buckling behavior of CNT arrays at the nanoscale will enable their improved design for high-strain electrical contacts, compliant thermal interfaces, force sensors, energy-absorbing foams, or other applications.