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To investigate the impact of diverse soil characteristics and surface irregularities on interfacial shear strength attributes, a large-scale straight shear apparatus and particle flow software were employed to conduct interfacial shear experiments with varying soil properties and surface irregularities. The results demonstrated that, under an identical R and normal stress conditions, the clay and silty clay shear stress–displacement curves exhibited strain softening, while the silt curve exhibited strain hardening. An increase in R can markedly enhance the peak shear strength at the interface, although a critical value exists beyond which this effect is no longer observed. The Rc is primarily contingent upon the soil properties. Numerical simulations demonstrate that the internal shear displacement and deformation resulting from the diverse soil properties are distinct. Clay particles are constituted of varying-sized particle aggregates that collectively resist shear. Silt particles resist shear through interfacial friction generated by shear. The practicality of Duncan and Clough’s constitutive model for interfacial shear with roughness influence is verified, and the constitutive model under strain hardening is modified.