A coatable polyvinylbutyral (PVB)-polyaniline (PANI) nanocomposite was designed for high microwave absorption efficiency. The maximum absorption efficiency 88.2 dB GHz/mm was obtained for the PANI nanofiber-loaded PVB (PVBPN) nanocomposite with a large bandwidth, whereas a pristine PANI-containing composite shows 53.5 dB GHz/mm in the frequency range 8.2-18 GHz. The presence of nanoslit pores in PVBPN also helps to achieve a large bandwidth and hence high microwave absorption efficiency. Standard electromagnetic simulation also shows that power absorbed by the PVBPN nanocomposite is high and its ultrathin coating over the dielectric substrate (epoxy) is promising for broadband tuneable reflection loss. © Copyright 2018 American Chemical Society.