Waste carbon nanotubes (CNTs) have always been a potential threat to the environment and biological health. However, the efficient recycling and utilization of CNTs has received little attention. Here, we used chemically cross-linked polyacrylamide (PAM) particles to adsorb waste CNTs in water to prepare PAM@CNT core-shell particles, which were blended with thermoplastic styrene-butadiene rubber (SBS) to prepare flexible composites. The concentration of residual CNTs in the supernatant was less than 3.5 μg mL−1, which meets the safety standards for discharge. The unique core-shell structure enables the composites with a thickness of 1 mm to exhibit high electromagnetic interference shielding effectiveness (53.3 dB) and low reflectivity (1.4 dB) at 30 wt% CNT content. In addition, at a CNT content of 10 wt%, the composites exhibit superior sensing properties concerning strain and solvents. Moreover, the composites prepared from different sources of waste CNTs have the same sensing properties. This work provides an effective strategy for the highly efficient recycling of waste CNTs for the preparation of green, high-performance multifunctional polymer composites for EMI shielding, human motion and solvent leakage monitoring, and solvent category differentiation.