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Abstract The convergence of proton conduction and multiferroics is generating a compelling opportunity to achieve strong magnetoelectric coupling and magneto-ionics, offering a versatile platform to realize molecular magnetoelectrics. Here we describe machine learning coupled with additive manufacturing to accelerate the design strategy for hydrogen-bonded multiferroic macromolecules accompanied by strong proton dependence of magnetic properties. The proton switching magnetoelectricity occurs in three-dimensional molecular heterogeneous solids. It consists of a molecular magnet network as proton reservoir to modulate ferroelectric polarization, while molecular ferroelectrics charging proton transfer to reversibly manipulate magnetism. The magnetoelectric coupling induces a reversible 29% magnetization control at ferroelectric phase transition with a broad thermal hysteresis width of 160 K (192 K to 352 K), while a room-temperature reversible magnetic modulation is realized at a low electric field stimulus of 1 kV cm −1 . The findings of electrostatic proton transfer provide a pathway of proton mediated magnetization control in hierarchical molecular multiferroics. 

Spin waves, quantized as magnons, have low energy loss and magnetic damping, which are critical for devices based on spin‐wave propagation needed for information processing devices. The organic‐based magnet [V(TCNE)x; TCNE = tetracyanoethylene; x ≈ 2] has shown an extremely low magnetic damping comparable to, for example, yttrium iron garnet (YIG). The excitation, detection, and utilization of coherent and non‐coherent spin waves on various modes in V(TCNE)x is demonstrated and show that the angular momentum carried by microwave‐excited coherent spin waves in a V(TCNE)x film can be transferred into an adjacent Pt layer via spin pumping and detected using the inverse spin Hall effect. The spin pumping efficiency can be tuned by choosing different excited spin wave modes in the V(TCNE)x film. In addition, it is shown that non‐coherent spin waves in a V(TCNE)x film, excited thermally via the spin Seebeck effect, can also be used as spin pumping source that generates an electrical signal in Pt with a sign change in accordance with the magnetization switching of the V(TCNE)x. Combining coherent and non‐coherent spin wave detection, the spin pumping efficiency can be thermally controlled, and new insight is gained for the spintronic applications of spin wave modes in organic‐based magnets.