Tungsten has many attractive properties, but its brittleness limits its application. Our team has found that the brittleness of tungsten can be greatly improved by combining the brittle tungsten with tantalum. Furthermore, we found that if a suitable transition layer is added between tungsten and tantalum, the properties of the composite will be further improved. In this paper, we studied the effect of different transition layers on the properties of W-Ta laminated composite to explore a suitable transition layer, which can effectively improve the toughness of the composite and solve the problem of tungsten application. We have prepared four kinds of W-Ta laminated composites with Ni, Ti, Nb, and Mo as transition layers. Ta-W laminated composites were prepared by stacking layers with Ta, transition layer, W alternately and sintered by spark plasma sintering (SPS). The tensile and three-point bending tests were carried to compare the mechanical properties. The tensile fracture morphology and three-point bending crack distribution were observed by SEM. In addition, the diffusion of elements in the transition layer and the influence of element diffusion on the tungsten structure were also studied to clarify the toughening mechanism. The results show that Nb is a satisfying transition layer, which not only improves the strength of W-Ta laminated composite, but also improves the toughness. The tensile test of W/Nb/Ta laminated composite shows a typical plastic fracture mode with an elongation of 13%. Three-point bending test also shows high strength and good toughness. In addition, Voigt model was used to predict the elastic modulus of W-Ta laminated composites and compared with the experimental results.