  Recent studies have shown that graphene-derived materials not only feature
outstandingly multifunctional properties, but also act as model materials to
implant nanoscale structural engineering insights into their macroscopic
performance optimization. Functionalizing the interfaces between graphene
sheets by interlayer crosslinks has been proven to be an effective route to
tune the mechanical properties. Here we explore the graphene-derived material
with a layer-by-layer structure and multiple crosslinking mechanisms. The
effects of multimodal and self-healable crosslinks are assessed in terms of
interlayer loading transfer capability. The results show that the
brick-and-motar hierarchy and synergetic effects from different crosslinks
enable synergetic enhancement in the strength and toughness. The findings here
could shed light on the development of high-performance paper-, fiber- or
film-like macroscopic materials from monolayer nanosheets with nanoengineerable
interfaces.
