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Memristive devices are under intense development as non‐volatile memory elements for extending the computing capabilities of traditional silicon technology by enabling novel computing primitives. In this respect, interface‐based memristive devices are promising candidates to emulate synaptic functionalities in neuromorphic circuits aiming to replicate the information processing of nervous systems. A device composed of Nb/NbOx/Al2O3/HfO2/Au that shows promising features like analog switching, no electro‐forming, and high current‐voltage non‐linearity is reported. Synchrotron‐based X‐ray photoelectron spectroscopy and depth‐dependent hard X‐ray photoelectron spectroscopy are used to probe in situ different resistance states and thus the origin of memristive switching. Spectroscopic evidence for memristive switching based on the charge state of electron traps within HfO2 is found. Electron energy loss spectroscopy and transmission electron microscopy support the analysis. A device model is proposed that considers a two‐terminal metal–insulator–semiconductor structure in which traps within the insulator (HfO2/Al2O3) modulate the space charge region within the semiconductor (NbOx) and, thereby, the overall resistance. The experimental findings are in line with impedance spectroscopy data reported in the companion paper (Marquardt et al). Both works complement one another to derive a detailed device model, which helps to engineer device performance and integrate devices into silicon technology. [ABSTRACT FROM AUTHOR]