With the explosive growth of electrocommunication and portable electronics, exploiting the superior electromagnetic interference (EMI) shielding materials with the desired flexibility and lightweight is critical. Herein, the waste carbon fibers (CFs) eco-friendly recycling strategy and a facile and cost-effective paper-making method are utilized to prepare recycled carbon fiber felt (rCFF) decorated with cationic polyacrylamide (CPAM) (rCFF/CPAM). Profiting from the inherent excellent conductivity of lossless recycled carbon fibers (rCFs) and optimum rCFs dispersion in CPAM, the abundant efficient pathways are constructed in the 3D interconnected rCFF/CPAM networks, resulting in the rCFF/CPAM exhibits a remarkable electrical conductivity of 140.06 S/m, a highly efficient EMI shielding effectiveness (EMI SE) of 66.15 dB and an exceptional of SEA/SET ratio of 83.8 % at 0.875 mm. More importantly, the felt also contains the advantages of outstanding flexibility, lightweight and sustainable re-utilization. In summary, this strategy provides an economical and practical way to manufacture the superior performance rCFF/CAPM, but also promotes the high value recycle and reuse of waste carbon fiber resources.