This study aimed to investigate the effect of different coating processes on interlayer coating using ProCAST software and identify the preferred coating process so as to prepare an EH40/2205 composite plate with a coating interlayer of Ni-5 Fe-15 Co (wt.%) displaying good performance. The preparation and characterization tests were conducted to analyze the interlayer coating, the diffusion of elements at the bonding interface and the mechanical properties of the hot-rolled composite plate. The results showed that the coating rate increased linearly with an increase in the initial coating temperature, pressure difference and the width ratio of the suction layer. The interlayer coating was complete under the guidance of optimized process parameters, and the test results and simulations confirmed each other. The coated interlayer successfully blocked the diffusion of elements between the bonding surfaces. The tensile strength of the rolled composite plate was 580 MPa, which met the needs of the project. The tensile shear fracture occurred at EH40, which proved that the plate was well bonded.