The present work reports an enhanced magnetoelectric (ME) effect at room temperature (RT) and above in a nanocomposite of LaYFe 2 O 6 /poly(vinylidene fluoride)−hexafluoropropylene [LaYFe 2 O 6 /P(VDF-HFP)], which is prepared by the solution-casting method. Field-emission scanning electron microscopy, X-ray diffraction, and Fourier transform infrared spectroscopy reveal excellent phase-to-phase connectivity and an enhanced beta-phase fraction in the PVDF matrix by the incorporation of 10 wt % antiferromagnetic nanoparticles (NPs). This is also substantiated by the improved ferroelectric (electric-field-dependent polarization) response by a 10 wt % sample. At RT, this nanocomposite manifests a first-order ME coupling coefficient of ∼2.92 mV cm −1 Oe −1 and a second-order ME coupling coefficient of ∼0.051 μV cm −1 Oe −2 (significantly 1 order higher than that of pristine LaYFe 2 O 6 ). The enhanced ME coefficient at RT and above makes it a viable candidate to address the challenges of ME-based device applications. A flexible, portable, lightweight, costeffective magnetoelectric nanogenerator (MENG) fabricated from the nanocomposite film is able to harvest the wasted magnetic energy with an efficiency of 1.5%. As a demonstration, the harvested electric energy is stored in a capacitor, which, in turn, is used to power a light-emitting diode (LED). The present work hence suggests the deployment of this material for self-powered wearable devices.