This paper describes a fully aqueous- and air-compatible chemical approach to preparing high-performance conductive textiles. In this method, the surfaces of textile materials are first modified with an aqueous solution of double-bond-containing silane molecules to form a surface-anchoring layer for subsequent in situ free-radical polymerization of [2-(methacryloyloxy)ethyl]trimethylammonium chloride (METAC) in the air. Thin layers of poly-METAC (PMETAC) are therefore covalently grafted on top of the silane-modified textile surface. Cu- or Ni-coated textiles are finally fabricated by electroless deposition (ELD) onto the PMETAC-modified textiles. Parameters including polymerization time, temperature, and ELD conditions are studied to optimize the whole fabrication process. The as-made conductive textiles exhibit sheet resistance as low as 0.2 Ω sq(-1) , which makes them highly suitable for use as conductive wires and interconnects in flexible and wearable electronic devices. More importantly, the chemical method is fully compatible with the conventional "pad-dry-cure" fabrication process in the textile manufacturing industry, thus indicating that it is very promising for high-throughput and roll-to-roll fabrication of high-performance metal-coated conductive textiles in the future.