In this paper, we report a cost-effective and scalable approach to produce highly homogeneous graphene and CNT-based silicone composites with potential applications in diverse fields of research, including biosensors and wearable electronics. This approach includes the fabrication of hybrid fillers based on few-layer graphene and CNTs by water solution blending and manufacturing of graphene/CNT/PDMS composites through calendering in a three-roll mill. The influence of processing parameters, the graphene/CNT ratio, and hybrid filler loading was thoroughly investigated, and the optimal parameters for producing hybrid composites with superior electrical and mechanical properties were found. It was also confirmed that the graphene/CNT hybrid system exhibits a synergistic effect of non-covalent interactions between graphene sheets and CNT sidewalls. This synergistic effect prevents the aggregation of graphene sheets, facilitates the dispersion of graphene and CNTs in the silicone matrix, and contributes to the superior properties of hybrid composites compared to composites with either of these fillers alone.

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