Atomic force microscopy (AFM), field-emission scanning electron microscopy, and energy dispersive X-Ray spectroscopy are used to study morphological and compositional variations of metal-organic interfaces in organic bistable devices. The results show that bias voltage causes rougher interfaces with new protrusions, and the switching phenomena origins from the evolution of these protrusions under external electric field. In order to exclude other possible factors, three types of bistable devices are designed and examined. In addition, metal-coated AFM probes are utilized to simulate the switching process, which yields similar results and corroborates our conclusion.