Structuralized cementing technology takes full advantage of non-pressure controlled grouting technology to fill pores in coarse aggregates using self-compacting material with no need for vibration or mixing. By cementing the aggregates in a structured manner, structurally cemented material has properties between those of a discrete granular material and a continuous medium. The interface between different component structures exerts an important effect on the physical properties of the whole material. In this paper, the monotonic and cyclic mechanical properties of the contact interface properties of a structurally cemented material under different normal stresses are studied by performing experiments and numerical simulations. Through the study, the deformation displacement time history and volume change with the shear process are provided, the deformation process of the sample near the contact interface during the shear process is discussed, and the shear mechanics law with the strength mechanism under the simple shear condition is summarized.