  The creation of multilayer graphene (Gr), while preserving the brilliant
properties of monolayer Gr derived from its unique band structure, can expand
the application field of Gr to the macroscale. However, the energy-favorable AB
stacking structure in the multilayer Gr induces a strong interlayer interaction
and alters the band structure. Consequently, the intrinsic properties of each
monolayer are degraded. In this work, we insert carbon nanotubes (CNTs) as
nanospacers to modulate the microstructure of multilayer stacking Gr.
Nanospacers can increase the interlayer distance and reduce the interlayer
interaction. The Gr/CNT stacking structure is experimentally fabricated using a
dry transfer method in a layer-by-layer manner. Raman spectroscopy verifies the
reduction in the interlayer interaction within the stacking structure. Atomic
force microscopy shows an increase in the interlayer distance, which can
explain the weakening of the interlayer interactions. The microstructure of the
stacked Gr and CNTs is studied by molecular dynamics simulation to
systematically investigate the effect of CNT insertion. We found that the
distribution distance, size, and arrangement of the CNT can modulate the
interlayer distance. These results will help us to understand and improve the
properties of the composite systems consisting of Gr and CNTs.
