Natural melanins are biocompatible conductors with versatile functionalities. Here, we report fabrication of multifunctional poly(vinyl alcohol)/melanin nanocomposites by layer-by-layer (LBL) assembly using melanin nanoparticles (MNPs) directly extracted from sepia officinalis inks. The LBL assembly offers facile manipulation of nanotextures as well as nm-thickness control of the macroscale film by varying solvent qualities. The time-resolved absorption was monitored during the process and quantitatively studied by fractal dimension and lacunarity analysis. The capability of nanoarchitecturing provides confirmation of complete monolayer formation and leads to tunable iridescent reflective colors of the MNP films. In addition, the MNP films have durable electrochemical conductivities as evidenced by enhanced charge storage capacities for 1000 cycles. Moreover, the MNP covered ITO (indium tin oxide) substrates significantly reduced secretion of inflammatory cytokines, TNF-α, by raw 264.7 macrophage cells compared to bare ITO, by a factor of 5 and 1.8 with and without lipopolysaccharide endotoxins, respectively. These results highlight the optoelectronic device-level tunability along with the anti-inflammatory biocompatibility of the MNP LBL film. This combination of performance should make these films particularly interesting for bioelectronic device applications such as electroceuticals, artificial bionic organs, biosensors, and implantable devices.

The development of electronic devices from naturally derived materials is of enormous scientific interest. Melanin, a dark protective pigment ubiquitous in living creatures, may be particularly valuable because of its ability to conduct charges both electronically and ionically. However, device applications are severely hindered by its relatively poor electrical properties. Here, the facile preparation of conductive melanin composites is reported in which melanin nanoparticles (MNPs), directly extracted from squid inks, form electrically continuous junctions by tight clustering in a poly(vinyl alcohol) (PVA) matrix. Prepared as freestanding films and patterned microstructures by a series of precipitation, dry casting, and post‐thermal annealing steps, the percolated composites show electrical conductivities as high as 1.17 ± 0.13 S cm−1 at room temperature, which is the best performance yet obtained with biologically‐derived nanoparticles. Furthermore, the biodegradability of the MNP/PVA composites is confirmed through appetitive ingestion by Zophobas morios larvae (superworms). This discovery for preparing versatile biocomposites suggests new opportunities in functional material selections for the emerging applications of implantable, edible, green bioelectronics.

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