Lamellar nanosheets of contrasting materials are ubiquitous in functional coatings and electronic devices. They also represent a unique paradigm for polymer nanocomposites. Here, we use fluid-assembled lamellar nanosheets - alternating layers of polymer and single-wall carbon nanotubes (SWCNTs) - to gain insight into the flexural mechanics of such hybrid films. Specifically, we measure the modulus and yield strain as a function of both layer thickness and the total number of layers. Overall, we find that the multi-layered films exhibit the greatest synergistic effects near a layer thickness of 20 nm or less, which we relate to the characteristic width of the SWCNT-polymer interface. For all layer thicknesses, we find that the nanosheets have realized the bulk limit by six layers. Our results have potentially profound implications for controlling the rigidity and durability of polymer nanocomposites, thin hybrid films and flexible heterojunctions.

Thin bilayers of contrasting nanomaterials are ubiquitous in solution-processed electronic devices and have potential relevance to a number of applications in flexible electronics. Motivated by recent mesoscopic simulations demonstrating synergistic mechanical interactions between thin films of single-wall carbon nanotubes (SWCNTs) and spherical nanocrystal (NC) inclusions, we use a thin-film wrinkling approach to query the compressive mechanics of hybrid nanotube/nanocrystal coatings adhered to soft polymer substrates. Our results show an almost 2-fold enhancement in the Young modulus of a sufficiently thin SWCNT film associated with the presence of a thin interpenetrating overlayer of semiconductor NCs. Mesoscopic distinct-element method simulations further support the experimental findings by showing that the additional noncovalent interfaces introduced by nanocrystals enhance the modulus of the SWCNT network and hinder network wrinkling.