Zhongxuan Wang, Yong Hu, Zhenyao Fang, Yixiao Wang, Peng Yan, Jiayue Sun, Mario Lopez, Ryan Stadel, Yuchen Niu, Joshua M. Little, Qimin Yan, Po-Yen Chen, Cheng Gong, Joseph W. Bennett, G D Gu, Qiang Li, Zhijie Chen, Taylor J. Woehl, Efrain E. Rodriguez, Kai Liu, Shenqiang Ren
. Molecular insertion reshapes the interfacial electrostatic environment, induces charge redistribution, and expands the interlayer spacing, resulting in enhanced ferroic order, including a 5-fold increase in magnetic anisotropy energy (0.35→1.6 meV/Fe) and strengthened ferroelectric polarization. The resulting chiral CIPS-FGT heterostructures exhibit robust room-temperature magnetoelectric coupling (∼4.8% magnetization modulation) and enable helicity-dependent control of ferroic states under circularly polarized light, producing a 54.4% resistance modulation. This work establishes molecular intercalation as a general strategy for engineering light-responsive 2D multiferroics for optically tunable magnetoelectric and spintronic devices.