Two-dimensional (2D) multiferroic materials with polarization-tunable electronic properties provide unprecedented opportunities for designing high-performance ferroelectric tunnel junctions (FTJs). In this work, we focus on ${\text{InCrS}}_3$, a 2D multiferroic derived from ferroelectric ${\text{In}}_2{\mathrm{S}}_3$ via Cr substitution, which exhibits a distinct polarization-modulated electronic phase transition, half-metallic in one polarization state and semiconducting in the other. Using density functional theory combined with the nonequilibrium Green’s function method, we reveal that the transport performance of ${\text{InCrS}}_3$-based FTJs is strongly dependent on the choice of electrode materials, originating from a momentum-selective coupling effect between the electronic states of electrodes and ${\text{InCrS}}_3$. When graphene is used as the electrode, the system exhibits an abnormal transport behavior: the metallic state shows ultralow transmittance due to momentum-space mismatch near the $\mathrm{K}$ point, while the semiconducting state shows much higher transmittance. In contrast, using metallic ${\text{NbS}}_2$ as the electrode restores normal transport behavior, as the electronic states overlap in momentum space around the $\mathrm{\Gamma }$ point. Our findings highlight that electrode selection can fundamentally alter the switching behavior of 2D FTJs and establish momentum matching as a key design principle for achieving high-contrast tunneling electroresistance in ferroelectric memory devices.

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• Electronic structure
• Quantum transport
• Ferroelectrics
• Janus materials
• Multiferroics
• Tunnel junctions
• van der Waals systems
• First-principles calculations