Using
the earth-abundant natural biomaterials to manufacture functional
electronic devices meets the sustainable requirement of green electronics,
especially for the practical application of memristors in data storage
and neuromorphic computing. However, the sneak currents flowing though
the unselected cells in a large-scale cross-bar memristor array is
one of the major problems which need to be tackled. The self-selecting
memristors can solve the problem to develop compact and concise integrated
circuits. Here, a sustainable natural biomaterial (anthocyanin, C15H11O6) extracted from plant tissue
is demonstrated for ions and electron transport. The capacitive-coupled
memristive behavior of as-prepared bioelectronic device can be significantly
modulated by diethylmethylÂ(2-methoxyethyl)Âammoium bisÂ(trifluoromethylsulfonyl)Âimide
(DEME-TFSI) ionic liquid (IL). Furthermore, graphene was inserted
into biomaterial matrix to manipulate the memristive effects by graphene
protonation. This results in a battery-like self-selective memristive
effect. This phenomenon is explained by a physical model and density
functional theory (DFT) based first-principles calculations. Finally,
the self-selective behavior was applied in 0T-1R array configuration,
which indicates the battery-like self-selecting biomemristor has potential
applications in the brain-inspired computing, data storage systems,
and high-density device integration.