To enable long-term progress, next-generation nonvolatile memories should function on the basis of new concepts that are different from the conventional charge storage in floating-gate transistors. [4][5][6] Of the emerging storage principles, electrically modulated resistive switching behaviors in metal-insulator-metal (MIM) structures could be an intriguing concept to redefine the frontiers of next-generation nonvolatile memories. [7][8][9][10][11][12][13][14] Such implementation offers promising advantages in several key aspects, including down-scalability, switching speed, power consumption, and fabrication cost.Resistive switching has been demonstrated in a wide variety of inorganic [7][8][9][10] and organic [11][12][13][14] materials, which are generally deposited as a continuous thin film sandwiched in between two conductive electrodes forming a MIM structure. However, careful consideration should be taken during the fabrication process, because deposition of these materials using various power-demanding methods (e.g., thermal evaporation, molecular beam epitaxy, and chemical vapor deposition) could possibly lead to an energy-imbalance situation. [15] Furthermore, utilization of materials derived from nonrenewable resources (e.g., mined minerals and fossil fuels) could raise critical issue regarding sustainability. In general, these materials are chemically robust and thus require an infinitely long period for natural decomposition after disposal, leaving behind massive volumes of electronic waste overwhelming landfills around the world. [16] In tandem with the growing environmental awareness and the proliferation of disposable electronics, there is an urgent need to develop more electronic applications based on the greener bio-organic materials, [16,17] which are generally derived from living (or once-living) organisms that are abundant in the nature. Bio-organic materials are not only biodegradable, biocompatible, and environmentally benign to provide a sustainable solution in addressing the environmental concerns, but also exotic for next-generation electronics realization. Recently, resistive switching behaviors demonstrated in several bio-organic MIM structures (Table S1, Supporting Information) have garnered considerable attention owing to their potentials as a plausible alternative for next-generation nonvolatile memories.Growing environmental awareness has prompted a paradigm shift toward using green materials for various electronic applications. Bio-organic materials are promising candidates attributable to their inherent biocompatibility, biodegradability, and environmental friendliness. Here, a nonvolatile memory device based on resistive switching in a bio-organic polysaccharides film is presented. The polysaccharides are extracted from natural Aloe vera gel using facile alcohol precipitation. Optimal film deposition is achieved through spin-coating followed by drying at 120 °C, which is higher than the usual processing temperature of commercial Aloe vera gel. Both bipolar and unipolar resistiv...