Chitosan has attracted significant attention in the past decade because of its potential applications in water engineering, the food and nutrition technology, the textile and paper industries, and drug delivery. Recently, a particularly interesting application of chitosan has been proposed in transparent flexible electronic devices, including memristors and transistors. In this work, the resistive switching (RS) effect of chitosan thin films in a capacitor-like structure with Ag and Al as alternative top electrodes was studied. Both the devices showed a bistable RS effect under an external electric field with a high endurance of 102. The electrical conduction and RS mechanisms of chitosan-based devices were investigated. The trap-controlled space charge–limited current was responsible for electrical transport at the low-resistance state of both devices, while direct tunneling and Schottky emission at the high-resistance state were related to Ag/chitosan/fluorine-doped tin oxide (FTO) and Al/chitosan/FTO, respectively. The RS mechanism of the Ag/chitosan/FTO device was attributed to the formation and dissociation of Ag filaments through the dielectric layer, whereas the change in the barrier height at the Al and chitosan interface under an external electric field could control the RS mechanism of the Al/chitosan/FTO device.