Magnetostrictive composite known as magnetostrictive nanocellulose membrances (MNMs) were fabricated by embedding Terfeonol-D particles into cellulose nanofibers (CNFs). MNMs inherit flexibility and biodegradability from CNF while exhibiting magnetomechanical responses; as such, the valuable rare-earth (Terfenol-D) particles can be recycled. Various orientations of the Terfenol-D particles were induced in the MNMs, and those with in-plane alignment showed the strongest magnetostrictive effect but the lowest Villari effect. Materials with such a unique combination of properties dovetail nicely with Internet of Things that require ubiquitous sensing, actuation, and energy harvesting in one package.