The Lianghekou earth core rockfill dam to be built in China will be the third highest rockfill dam in the world. This study presents the results of a series of direct shear tests between high plastic clay and concrete to study the shear behavior of contact clay-concrete cushion interface of Lianghekou dam. Results showed that water content and normal stress are significant factors affecting the shear behavior of the interface. The higher shear strength is related to lower water content and higher normal stress, and the shear strength can be formulated by the bifold-line type Mohr–Coulomb strength criterion. It is also found that the interface exhibits mainly two kinds of shear failure modes, that is, sliding failure along the concrete surface and shear failure in the clay matrix nearby the interface. Moreover, a nonlinear elastic model is proposed to simulate the shear behavior of the interface, of which parameters can be quickly estimated by water content. The simulation of the model is compared with the experimental results, and the results show that the model is reasonable and practical.