As modern electronics advance toward miniaturization
and integration,
there is an increased demand for effective thermal management solutions.
One of the most promising strategies to achieve this is to enhance
the thermal transport capacity of thermal interface materials (TIMs)
by incorporating fillers. In this study, carbon fiber was used as
the framework, and a simple shear stress-oriented approach was employed
to orient graphene flatly onto the carbon fiber surface, yielding
high thermal conductivity ordered carbon fiber and graphene (OCF/G)
films. A sandwich-structured thermal interface material was fabricated
by vertically embedding laser-processed optical fibers (OCF/G) into
a silicone gel matrix. The vertically arranged OCF/G films, as the
heat transfer path, retained their high thermal conductivity, while
the interconnected silicone gel network offered superior mechanical
properties. The through-plane thermal conductivity of the composites
is 37.26 W m–1 K–1, which is 226
times higher than pure PDMS and 68 times higher than the composite
with only carbon fibers loading. Additionally, thermal management
applications of the composites as thermal interface materials for
electronic device cooling are demonstrated. This construction method
provides an effective approach for designing thermal interface materials
with enhanced thermal and mechanical performance.