Achieving electrical control of magnetic states is highly pursued for next-generation nonvolatile memory, yet it remains a significant challenge in spintronic devices. In this study, we propose a homojunction-based strategy to realize fully electrical control of spin valve. We demonstrate that the multiferroic α-MXenes ${\mathrm{Cr}}_2{\mathrm{CO}}_2$ and ${\mathrm{Mn}}_2{\mathrm{CO}}_2$ exhibit not only ferromagnetic half-metallicity with high Curie temperatures but also a moderate ferroelectric dipole moment with feasible polarization-switching barriers. Owing to the robust magnetoelectric coupling effect, the ferromagnetic and antiferromagnetic states in ${\mathrm{Cr}}_2{\mathrm{CO}}_2/{\mathrm{Cr}}_2{\mathrm{CO}}_2$ and ${\mathrm{Mn}}_2{\mathrm{CO}}_2/{\mathrm{Mn}}_2{\mathrm{CO}}_2$ homojunctions can be toggled by switching their own polarization directions. To elucidate the underlying electric control mechanism, we constructed two spin valve devices with the following layered structures: 1T-${\mathrm{MoS}}_2/{\mathrm{Cr}}_2{\mathrm{CO}}_2/{\mathrm{Cr}}_2{\mathrm{CO}}_2$/1T-${\mathrm{MoS}}_2$ and 1T-${\mathrm{MoS}}_2/{\mathrm{Mn}}_2{\mathrm{CO}}_2/{\mathrm{Mn}}_2{\mathrm{CO}}_2$/1T-${\mathrm{MoS}}_2$. Remarkably, these spin valves exhibit engineered interfacial contacts and achieve a fully electrically controlled magnetoresistance ratio (MR) of $\sim {10}^6\%$, benefiting from the distinctive junction properties and precisely tailored architecture. This study not only provides a perspective for the development of electrical writing and magnetic reading nonvolatile memory but also provides insights for designing other advanced spintronic devices.

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• Ferroelectricity
• Magnetism
• Interfaces
• Density functional theory