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This paper reports the fabrication and mechanical properties of macroscale graphene fibers (diameters of 10 to 100 μm with lengths upwards of 2 cm) prepared from a single sheet of single-layer graphene grown via chemical vapor deposition (CVD). The breaking strength of these graphene fibers increased with consecutive tensile test measurements on a single fiber, where fiber fragments produced from a prior test exhibited larger breaking strengths. Additionally, we observed an overall reduction of surface folds and wrinkles, and an increase in their alignment parallel to the tensile direction. We propose that a foundation of this property is the plastic deformations within the fiber that accumulate through sequential tensile testing. Through this cyclic method, our best fiber produced a strength of 2.67 GPa with a 1 mm gauge length. 

Abstract Smart materials are versatile material systems which exhibit a measurable response to external stimuli. Recently, smart material systems have been developed which incorporate graphene in order to share on its various advantageous properties, such as mechanical strength, electrical conductivity, and thermal conductivity as well as to achieve unique stimuli‐dependent responses. Here, a graphene fiber‐based smart material that exhibits reversible electrical conductivity switching at a relatively low temperature (60 °C), is reported. Using molecular dynamics (MD) simulation and density functional theory‐based non‐equilibrium Green's function (DFT‐NEGF) approach, it is revealed that this thermo‐response behavior is due to the change in configuration of amphiphilic triblock dispersant molecules occurring in the graphene fiber during heating or cooling. These conformational changes alter the total number of graphene‐graphene contacts within the composite material system, and thus the electrical conductivity as well. Additionally, this graphene fiber fabrication approach uses a scalable, facile, water‐based method, that makes it easy to modify material composition ratios. In all, this work represents an important step forward to enable complete functional tuning of graphene‐based smart materials at the nanoscale while increasing commercialization viability.