We report a systematic study of the linear magnetoelectric effect in $\mathrm{C}{\mathrm{o}}_4\mathrm{N}{\mathrm{b}}_2{\mathrm{O}}_9$ single crystals under pulsed magnetic fields up to 52 T. By applying sufficiently high magnetic and electric fields synergistically, a complete single-domain state is stabilized, enabling access to the intrinsic magnetoelectric response. Based on this, comprehensive field-dependent polarization measurements were performed along both $P_x$ ($x\parallel \left[110\right]$) and $P_y$ ($y\parallel [1-10]$) under various magnetic field orientations, yielding $\mathrm{\Delta }{P}_x\sim 1000\mu \mathrm{C}/{\mathrm{m}}^2$ and $\mathrm{\Delta }{P}_y\sim 110\mu \mathrm{C}/{\mathrm{m}}^2$, which allows determination of the dominant linear magnetoelectric tensor components ${\alpha }_{xx}, {\alpha }_{xy}, {\alpha }_{yx}$, and ${\alpha }_{yy}$. The angular-dependent polarization measurements reveal a periodic modulation of the linear magnetoelectric response in both multidomain and single-domain states, demonstrating that the polarization direction continuously follows the rotation of the magnetic moments under a rotating magnetic field.

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• Electric polarization
• Magnetoelectric effect
• Multiferroics