Single-crystalline Ni3Al-based superalloys have been widely used in aviation, aerospace, and military fields because of their excellent mechanical properties, especially at extremely high temperatures. Usually, single-crystalline Ni3Al-based superalloys are welded together by a Ni3Al-based polycrystalline alloy via transient liquid phase (TLP) bonding. In this study, the elastic constants of single-crystalline Ni3Al were calculated via density functional theory (DFT) and the elastic modulus, shear modulus, and Poisson’s ratio of the polycrystalline Ni3Al were evaluated by the Voigt–Reuss approximation method. The results are in good agreement with previously reported experimental values. Based on the calculated mechanical properties of single-crystalline and polycrystalline Ni3Al, three-dimensional finite element analysis (FEA) was used to characterize the mechanical behavior of the TLP bonded joint of single-crystalline Ni3Al. The simulation results reveal obvious stress concentration in the joint because of the different states of crystal orientation between single crystals and polycrystals, which may induce failure in the polycrystalline Ni3Al and weaken the mechanical strength of the TLP bonded joint. Furthermore, results also show that the decrease in the elastic modulus of the intermediate layer (i.e., polycrystalline Ni3Al) can relieve the stress concentration and improve the mechanical strength in the TLP bonded joint.