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Gallium‐based liquid metal (LM) composite with metallic fillers is an emerging class of thermal interface materials (TIMs), which are widely applied in electronics and power systems to improve their performance. In situ alloying between gallium and many metallic fillers like copper and silver, however, leads to a deteriorated composite stability. This paper presents an interfacial engineering approach using 3‐chloropropyltriethoxysilane (CPTES) to serve as effective thermal linkers and diffusion barriers at the copper‐gallium oxide interfaces in the LM matrix, achieving an enhancement in both thermal conductivity and stability of the composite. By mixing LM with copper particles modified by CPTES, a thermal conductivity (κ) as high as 65.9 W m⁻¹K⁻¹is achieved. In addition, κ can be tuned by altering the terminal groups of silane molecules, demonstrating the flexibility of this approach. The potential use of such composite as a TIM is also shown in the heat dissipation of a computer central processing unit. While most studies on LM‐based composites enhance the material performance via direct mixing of various fillers, this work provides a different approach to fabricate high‐performance LM‐based composites and may further advance their applications in various areas including thermal management systems, flexible electronics, consumer electronics, and biomedical systems.