This study aims to convert composite textile structures composed of nonwoven and woven fabrics produced from cotton–jute wastes into activated carbon textile structures and investigate the possibilities of using them for electromagnetic shielding applications. To this end, the novel contribution of this study is that it shows that directly carbonized nonwoven textile via self-purging microwave pyrolysis can provide Electromagnetic Interference (EMI) shielding without any processing, including cleaning. Textile carbonization is generally achieved with conventional heating methods, using inert gas and long processing times. In the present study, nonwoven fabric from cotton–jute waste was converted into an activated carbon textile structure in a shorter time via microwaves without inert gas. Due to its polar structure, FeCl3 has been used as a microwave absorbent, providing homogeneous heating in the microwave and acting as an activating agent to serve dual purposes in the carbonization process. The maximum surface area (789.9 m2/g) was obtained for 5% FeCl3. The carbonized composite textile structure has a maximum of 39.4 dB at 1 GHz of EMI shielding effectiveness for 10% FeCl3, which corresponds to an excellent grade for general use and a moderate grade for professional use, exceeding the acceptable range for industrial and commercial applications of 20 dB, according to FTTS-FA-003.