functionality of LM composites relies on assembly and interactions between the matrix and filler. [11,23,24] To date, most of these LM composites have utilized silicone rubbers, where the functionality imparted by the matrix is limited to mechanical compliance and deformability, although a few meaningful exceptions exist (e.g., where the LM catalyzes/initiates poly mer ization). [19,21,25,26] Synthetic polymers can be designed with properties like stimuli responsivity, self-healing, processability, shape-morphing, and dynamic compliance and could be combined with LM to permit novel functionalities and processing capabilities. [27] The combination of finely tuned polymer synthesis with LM composite engineering will enable advanced applications like soft prosthetics, self-healing artificial skins, and 3D electronic materials. To achieve electrical conductivity, LM droplets within a composite must coalesce, for example, through an applied pressure (termed "mechanical sintering"). [28] Notably, the curing conditions and precursor composition dictate the network topology and resulting mechanical properties of the silicone matrix, which appear to influence whether an applied pressure forms percolation pathways for a LM composite. For example, LM composites using a commercially available silicone formulation (Sylgard 184, 10:1 weight ratio of Part A and Part B) can be electrically conductive after application of localized pressure [28] that coalesces LM droplets. However, permanent electrical conductivity has not been observed in LM composites that use a different commercially available silicone formulation (Ecoflex 00-30, 1:1 weight ratio of Part A and Part B), which is softer and more deformable than Sylgard 184. [8,20,29] This difference poses a limitation in generality of functionality for LM composites. Progress in LM composite engineering depends on a framework for materials synthesis that overcomes this limitation and enables integration of electrically conductive networks of LM in a wider range of media. Importantly, progress toward multifunctionality should include a focus on the properties of the matrix material. For LM composites, our group and others have demonstrated LM incorporation in functional matrix materials like hydrogels and shape-morphing polymers, but the predominate choice of matrix material has been silicone rubbers. [19,21,25,26] The development of an approach to achieve electrical conductivity by incorporating LM in functional polymer networks will facilitate Soft composites that use droplets of gallium-based liquid metal (LM) as the dispersion phase have the potential for transformative impact in multifunctional material engineering. However, it is unclear whether percolation pathways of LM can support high electrical conductivity in a wide range of matrix materials. This issue is addressed through an approach to LM composite synthesis that focuses on the interrelated effects of matrix curing/solidification and droplet formation. The combined influence of LM concentration, particle size, and ...