The expanding realm of high‐frequency electronics necessitates materials with exceptional attributes: notably, a low dielectric constant (Dk) to minimize signal propagation delays, high thermal conductivity for effective heat dissipation, higher breakdown strength, and robust mechanical properties to withstand demanding operational environments. While cycloolefin copolymers (COC) excel in electrical insulation, chemical resistance, and mechanical durability, their intrinsic slightly higher dielectric constant compared to other polymers, along with challenges such as poor dispersibility and low compatibility with nanoparticles, hinder their full potential in this domain. Considering these drawbacks, this study fabricated a series of COC/mica composites by integrating natural mica particles into the COC matrix via a CTAB‐assisted surface modification of mica to enhance dispersibility and mitigating particle aggregation through in‐situ mixing and hot‐press methods. The resultant composites demonstrate an outstanding ultra‐low Dk of 1.44, marking a significant decrease of over 36% compared to pristine COC with a Dk of 2.26, along with exceptionally low dielectric loss (δ) of 0.00013 at the frequency of 10 GHz, high dielectric breakdown strength ~49.40 kV/mm and enhanced thermal conductivity up to 0.88 W/(m K) at 40% mica loading. Additionally, the composites heightened mechanical performances like tensile strength 69 MPa at 6.5% elongation at break, impact strength up to ~17.9 kJ × m−2, and exceptional water resistance with absorption below 0.097%. These exceptional ultra‐low dielectric performance with above mentioned properties can meet the stringent requirements of modern high‐frequency electronics packaging for next generation electronics development.Highlights
Surface modification by CTAB enhanced homogeneous dispersibility of composites.
Achieved ultra‐low dielectric constant and loss compared to pure COC.
Thermal conductivity improved significantly with incorporation of mica.
Unlocking high‐frequency applications potential with ultralow Dk performance.