Magnetoelectric (ME) materials face challenges in terms of practical applications and understanding of the underlying mechanisms of some phenomena. Studying these phenomena in glassy systems may provide fresh insights, but research along these lines remains limited. Our study reveals the existence of a glassy state at high temperature in single-crystal $\mathrm{FeNiM}{\mathrm{o}}_3{\mathrm{O}}_8$ (FNMO), providing a unique perspective for comprehending other high-temperature physical phenomena in this system. Remarkably, FNMO exhibits enhanced ME coupling, achieving the ME effect at elevated temperatures relative to other members of the $M_2{\mathrm{Mo}}_3{\mathrm{O}}_8$ family, and coupling with a higher second-order ME coefficient than its parent phase. Our research establishes a direct relation between the ME effect and the glassy state. The emergence of exchange bias in FNMO is controlled by the spin coupling at the interface between the glassy state and the antiferromagnetic state, opening up novel pathways for developing high-performance magnetic memories by using single-phase materials.

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• Magnetic interactions
• Magnetic phase transitions
• Crystal structures
• Ferroelectrics
• Multiferroics
• Spin glasses
• Crystal growth
• Dielectric constant measurements
• Dielectric spectroscopy
• Electron diffraction
• Focused ion beam
• Magnetization measurements
• X-ray diffraction