Carbon fiber (CF) laminates based on an engineering thermoplastic matrix, specifically polyetheretherketone (PEEK)/CF, are actively being investigated for their potential applications in aircraft structures. These laminates offer notable advantages, including high damage tolerance, weldability, elevated temperature performance, recyclability, and faster production rates when compared to traditional thermoset matrix-based CF laminates. These attributes position them as promising candidates for structural applications in aircraft. In addition to their structural properties, functional aspects such as deicing/anti-icing capabilities and electromagnetic interference (EMI) shielding are crucial for these aerospace applications. The ice accumulation at high altitudes during in-service flights poses a significant challenge, affecting aerodynamics and adding weight. Electrothermal heating stands out as a viable solution for deicing aerostructures. However, the inherent low electrical and thermal conductivity of the laminates poses a hurdle. While CFs exhibit excellent conductivity, the insulating polymer hinders both charge and thermal transport across the laminates. This study focuses on enhancing the transport properties of PEEK/CF laminates by integrating a stainless-steel (SS) mesh, thereby improving the electrothermal heating characteristics. The SS/PEEK/CF structure is engineered to enhance electrothermal heating, reducing the ice-melting time while preserving the mechanical properties of the laminate. To address the challenge of poor bonding between SS and PEEK, poly(ether imide) (PEI) is introduced due to its compatibility with the PEEK matrix. The incorporation of PEI-coated SS results in a notable improvement in interlaminar shear strength (ILSS), flexural strength (FS), and storage modulus-exhibiting enhancements of 9, 16, and 44%, respectively. The maximum temperature on the laminate surface increases from 41 to 92 °C, and deicing time decreases from 120 to 45 s with a modest applied voltage of 2 V. Furthermore, the electromagnetic interference (EMI) shielding effectiveness shows an increase from 47 to 60 dB. This unique structural approach, involving the incorporation of a metallic mesh and enhancing its bonding with the matrix, holds great promise for advancing aerostructures in terms of both performance and functionality.