Expanding resistive random-access memory (RRAM) from a single device to an array requires a selector to suppress the sneak path and an external device to control the compliance current. Thus, a unique crossbar array that can be independently driven through the novel design of a multilayer RRAM structure with intelligently controlled Cu2O consisting of nanoparticles embedded in the amorphous matrix (ANPs) is proposed. The ANPs–Cu2O active layers are prepared by electrodeposition, and the negative shift of the deposition potential induces a higher density and smaller size of the nanoparticles. The ANPs–Cu2O films show different set voltages and extremely uniform reset voltages, and thus a functional double active layer (DAL) structure consisting of two ANPs–Cu2O layers with different set voltages is proposed. The electrochemically fabricated VCu-controlled DALs effectively protected the reverse current from the self-rectifying characteristics of a large forward/reverse current ratio, thus realizing selector-less RRAMs. In addition, the soft-breakdown showing filament formation in the upper layer reveals the saturation current step acting as a self-compliance current without the assistance of transistors. Finally, a 4 × 4 crossbar DAL RRAM array with transistor-less self-rectification is demonstrated, which shows excellent memory performance and endurance without interfering with adjacent cells.