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Phototunable biomaterial‐based resistive memory devices and understanding of their underlying switching mechanisms may pave a way toward new paradigm of smart and green electronics. Here, resistive switching behavior of photonic biomemory based on a novel structure of metal anode/carbon dots (CDs)‐silk protein/indium tin oxide is systematically investigated, with Al, Au, and Ag anodes as case studies. The charge trapping/detrapping and metal filaments formation/rupture are observed by in situ Kelvin probe force microscopy investigations and scanning electron microscopy and energy‐dispersive spectroscopy microanalysis, which demonstrates that the resistive switching behavior of Al, Au anode‐based device are related to the space‐charge‐limited‐conduction, while electrochemical metallization is the main mechanism for resistive transitions of Ag anode‐based devices. Incorporation of CDs with …