The realization of artificial synapses based on biomaterials is of great significance for the development of environmentally friendly neuromorphic hardware systems and artificial intelligence. In this sense, a bioartificial synapse composited with egg albumen (EA) and multiwalled carbon nanotubes (MWCNTs) is fabricated. Based on the adjustable weight of the artificial synapse, the plasticity of electrical synapses is explored. Due to the photogenerated carriers and thermoelectric effects of carbon nanotubes, the device has optoelectronic properties, so the optoelectronic synaptic plasticity of the device is explored under light pulses. The device is well suited for biological synapses and shows great potential for applications in future high‐density storage and neuromorphic computing systems. In addition, to further study the physical mechanism of the conductive process of the device, the electrical characteristics of the contact interface between carbon nanotubes doped with Fe substitution and the upper electrode Al are mainly analyzed by first principles, and the adsorption, charge distribution, and band structure between them are theoretically studied.