AbstractThe small strain characteristics of the traditional flexible conductive composites hinder their realization of skin‐like properties and multi‐scenario applications. The value of liquid metal (LM)‐based elastomers is demonstrated in flexible electronics. Attempts in this area include the development of multifunctional LM‐based elastomers with controllable morphology, superior mechanical performances, and excellent stability. In this work, an efficient strategy is proposed to achieve the fast preparation of the LM patch by uniformly distributing eutectic gallium–indium–tin alloy in deionized water and by constructing the LM‐iron particles‐Ecoflex (LMIE) ternary composite system. In this study, the fabricated LMIE large strain sensor exhibits high sensitivity (the gage factor (GF) = 0.98 when strain ranges from 0% to 60%; GF = 1.91 when strain ranges from 60% to 100%), high linearity (correlation coefficient (R2) = 0.96 when strain ranges from 0% to 60%; R2 = 0.99 when strain ranges from 60% to 100%), a wide strain range of detection (e.g., 1%–100%) and breaking elongation (e.g., 450%), a fast response time (80 ms), excellent repeatability and stability. This work exhibits the excellent potential of multifunctional liquid metal composites in wearable electronics and prediction devices of structural collapse.