Laminated composites show great promise for achieving substantial magnetoelectric (ME) coupling through the manipulation of magnetostriction and piezoelectric engineering. However, the ME coupling mechanism in composites is less understood due to complex extrinsic effects at the interfaces, unlike the well-understood ME mechanism in chemically single-phase compounds. Our study reveals unexplored ferroelectric (FE) orders along $c$-axis and magnetostriction-driven ME couplings, indicating type-II multiferroic order in ${\mathrm{TbFeO}}_3$ and providing insight into the controversy surrounding ferroelectricity in $R{\mathrm{FeO}}_3$ orthoferrites. Neutron and synchrotron x-ray diffraction (SXD) results indicate exchange striction-driven FE order below 200 K, with Tb order leading to ferroelectricity below 3 K. SXD results also reveal significant magnetostriction along the $c$-axis, correlating with ME coupling at both FE orders. These findings directly demonstrate magnetostriction-driven ME coupling, and they suggest it as one of the potential mechanisms underlying ME coupling in multiferroics.

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• Magnetoelectric effect
• Magnetostriction
• Ferroelectrics
• Multiferroics
• Neutron diffraction
• X-ray diffraction