This Communication presents the important finding that certain chalcogenide materials, well-known from rewritable optical recording, allow resistive memory states that are a combination of two electrically-induced (reversible) switching processes, i.e., an actual amorphous-crystalline phase transformation and a (electrolytic) polarity-dependent resistance change. Nanometer-sized crystalline marks were written electrically in amorphous Ge 2 Sb 2+x Te 5 films using atomic force microscopy (AFM), and their resistance was found to depend on the polarity of the applied voltage with a resistance difference of three orders of magnitude. However, no contrast in current has been detected between the crystalline higherresistance state and the surrounding amorphous phase. This resistance switching is reversible for bias voltages well below the threshold voltage required to induce the phase transformation. The switching mechanism is attributed to the solidstate electrolytic behavior due to the presence of excess Sb in the films. Our results render exciting technological opportunities for data storage and encryption by combining both switching concepts.Following his seminal work in 1968, [1] Ovshinsky demonstrated in chalcogenide alloys a fast reversible transformation between amorphous and crystalline phases induced by electrical or optical (laser) pulses. [2][3][4] The two phases exhibited clear contrast in electrical and optical properties and, hence, these materials were suggested for binary data-storage applications. However, it took considerable time before rewritable optical compact discs (CD) and digital versatile discs (DVD) based on these findings came to the market. In recent years, the main focus of phase-change data-storage research returned to resistance switching. So-called chalcogenide or phase-change random access memory (CRAM/PRAM) and ovonic unified memory (OUM) based on the phase-dependent resistance switching are currently under intense investigations, [5][6][7][8][9][10][11][12][13] because they show great promise as next-generation nonvolatile solid-state memory replacing flash memory. In certain chalcogenides a special phenomenon of polaritydependent resistance switching (induced by an electric field) has been identified. [14][15][16][17][18][19] This is related to the solid-state electrolytic character and high ionic conductivities of chalcogenides, and hence is called ionic/electrolytic switching. For one polarity, the chalcogenide medium is electrically conductive by forming conducting filamentary pathways between electrodes, whereas for the reverse polarity it becomes relatively insulative or at least less conductive because of rupture of the previously formed electrical pathways. Memory elements (or structures) based on this switching have been demonstrated in some Ag-saturated chalcogenides including Ag-S, [14,15] AgGe-Se, [16,17] Ag-Ge-Te, [18] and Ag-In-Sb-Te. [19] This switching seems more attractive for applications than phase-dependent switching, because i) it can be performed at lower volta...