High electrical conductivity and electrical stability play a significant role in building the component devices of wearable electronics textiles. In this study, an implementable and effective approach was established that involved successive steps of surface microdissolution and in situ polymerization of pyrrole on fabric surfaces. The cotton fabrics were pretreated using a NaOH/urea aqueous solution system at low temperature so as to add more adsorption sites to the surface and obtain a rough surface. Then more polypyrrole was firmly deposited on the surface of the cotton fabrics. The results showed that the treated fabrics had a lower surface resistance of 1.98 Ω/sq, and the value was almost unchanged after 10 washing cycles. The dry rubbing fastness degree of the treated fabrics can reach 4 grades, and good flexibility was maintained under different bending states. Higher electromagnetic shielding effectiveness of the treated cotton fabrics (15.4–62.9 dB) at a frequency range from 1 to 3000 MHz and excellent ultraviolet protection performance could be obtained, which can provide a theoretical reference for the design and research of flexible wearable electrode materials. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47515.