Buckling patterns are universal in organs of living organisms. Moreover, the functional realization of these organs is precisely dependent on the deformation of buckling structures, which is also related to the effect of interfacial interaction between liquid and solid surfaces. However, the detection of synergistic reaction between the buckling pattern and the effect of liquid–solid interface is absent. Herein, an experimental simulation of buckling behaviors at the solid–liquid interface, that is, by depositing Au atoms on liquid polydimethylsiloxane (PDMS) is developed. Buckling patterns can be directly created at the interface of Au atoms film and liquid PDMS. Furthermore, it is demonstrated that the orientation of buckling structures can be strictly controlled depending on the frame edges placed on the surface of the liquid PDMS before the deposition. Various ordered buckling patterns, such as parallel wrinkles pattern, magnetic‐field‐lines‐like buckling pattern, and bionic patterns, can be prepared depending on this buckling behavior. The experimental simulation of the buckling behavior at the liquid–solid interface is well promoted, which may be further helpful in understanding the effect of interfacial interaction between liquid and solid surfaces.