Common pursuits of developing nanometric logic and neuromorphic applications have motivated intensive research studies into low-dimensional resistive random-access memory (RRAM) materials. However, fabricating resistive switching medium with inherent stability and homogeneity still remains a bottleneck. Herein, we report a self-assembled uniform biphasic system, comprising low-resistance 3 nm-wide (Bi 0.4 ,La 0.6 )FeO 3−δ nanosheets coherently embedded in a high-resistance (Bi 0.2 ,La 0.8 )FeO 3−δ matrix, which were spinodally decomposed from an overall stoichiometry of the (Bi 0.24 ,La 0.76 )FeO 3−δ parent phase, as a promising nanocomposite to be a stable and endurable RRAM medium. The Bi-rich nanosheets accommodating high concentration of oxygen vacancies as corroborated by X-ray photoelectron spectroscopy and electron energy loss spectroscopy function as fast carrier channels, thus enabling an intrinsic electroforming-free character. Surficial electrical state and resistive switching properties are investigated using multimodal scanning probe microscopy techniques and macroscopic I−V measurements, showing high on/off ratio (∼10 3 ) and good endurance (up to 1.6 × 10 4 cycles). The established spinodal decomposition-driven phase-coexistence BLFO system demonstrates the merits of stability, uniformity, and endurability, which is promising for further application in RRAM devices.