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This paper reports the generation of 3D thermal and electrical conductive graphene network in gallium‐based liquid metal (LM) via a simple one‐step ball‐milling approach. In this work, 2D graphene nanoplates and their derivatives were employed to construct 3D thermal and electrical conductive filler networks. It is demonstrated that the obtained composite exhibits the highest 3D thermal conductivity (44.6 W m−1 K−1) among the other gallium‐based LM composites with 2D inorganic nanofillers and distinguished electrical conductivity (8.3 S µm−1) among gallium‐based LM composites at present. The enhanced thermal conductivity and wettability of gallium‐based composite lead to its beneficial usage as thermal interface materials with exquisite texture for LED chip heat dissipation. The electrochemical and magnetic experiments confirm that these LM‐based composites can also be controlled under external electrical or magnetic field, which potentially can help extend their application in external field‐driven systems. The findings of this work offer new insight in designing LM‐based composites with enhanced thermal, electrical, and magnetic properties for a wide range of applications, including thermal management systems, 3D printing, flexible conductors, soft robotic systems, and wearable energy technologies. [ABSTRACT FROM AUTHOR]