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Miniaturization of individual selectors in crossbar‐array‐based artificial neural networks is essential for the advancement of the underlying neuromorphic electronics, as it improves learning, recognition, and prediction accuracies. This study proposes a tilt‐engineered molecular‐scale selector comprising a heterostructure of biphenyl‐4‐thiol (OPT2) or 1‐octanethiol (C8) molecular layers and an n‐type...