In view of the depletion of natural energy resources, harvesting energy from waste is a revolution to simultaneously capture, unite, and recycle various types of waste energies in flexible devices. Thus, in this work, a spin-charge-regulated pyro-magnetoelectric nanogenerator is devised at a well-known ferroelectric P(VDF-TrFE) copolymer. It promptly stores thermal-magnetic energies in a "capacitor" that generates electricity at room temperature. The ferroelectric domains are regulated to slip at the interfaces (also twins) of duly promoting polarization and other properties. An excellent pyroelectric coefficient p ∼ 615 nC•m −2 •K −1 is obtained, with duly enhanced stimuli of a thermal sensitivity ∼1.05 V•K −1 , a magnetoelectric coefficient α me ∼8.8 mV•cm −1 •Oe −1 at 180 Hz (resonance frequency), and a magnetosensitivity ∼473 V/T. It is noteworthy that a strategy of further improving p (up to 41.2 μC•m −2 •K −1 ) and α me (up to 23.6 mV•cm −1 •Oe −1 ) is realized in the electrically poled dipoles. In a model hybrid structure, the spins lead to switch up the electric dipoles parallel at the polymer chains in a cohesive charged layer. It is an innovative approach for efficiently scavenging waste energies from electric vehicles, homes, and industries, where abundant thermal and magnetic energies are accessible. This sustainable strategy could be useful in next-generation self-powered electronics.