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The FCC + BCC dual-phase solid solution structure was obtained in the Al0.1CoCrFeNi /304SS brazed joints using Ni/Al reactive multilayer nano-foils, which was proved by combining experiment with simulation. In this study, Finite Element Analysis was achieved to analyzing the diffusion behavior across brazing joints, which were subsequently interrelated with the formation mechanism of the brazed micro-structures during the brazing process. During brazing, the joint interface is tightly bonded and the atoms were diffused sufficiently to form the solid solution zone. The representative microstructure of the joint mainly comprised hard BCC (Al-Ni) + ductile FCC (Co-Fe-Cr) dual-phase. The successful use of nano-multilayer foils as a HEAs fillers design can broaden the application range of HEAs and provide a novelty procedure for brazing 304SS and Al0.1CoCrFeNi HEAs, and is developing a novel field in manufacture of HEAs-related joints.