Recent advancements in electronics and telecommunication require materials with excellent resiliency and sustainability in order to extend their lifetime. Keeping this in mind, we developed a sustainable multifunctional nanocomposite by combining the shape memory assisted self-healing (SMASH) capability of "mussel-inspired"dopamine functionalized polyurethane (PU) with synergistic electromagnetic interference (EMI) shielding capabilities from multiwalled carbon nanotubes (MWNTs) and ferrite doped with MoS2 (Fe3O4@MoS2). The self-healing ability in the polymer was driven by the reversible dynamic coordination bonds, between Fe3+ ions and hydroxyl functional groups of dopamine. The modified PU was also found to be capable of undergoing SMASH by heating it to 50 °C, whereby no manual intervention was required to bring the damaged ends together to trigger healing ability. The developed polymer and its nanocomposites performed quite well in terms of restoration of up to 75% and 56% of its original tensile strength, respectively. The nanocomposite showed outstanding EMI shielding capability of up to -36.6 dB manifesting in up to 96% absorption of EM waves. This strategy aims to shed some light on the design and development of sustainable and resilient materials for EMI shielding applications. Copyright © 2019 American Chemical Society.