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Due to the low electrical power generation in liquid cultures of photosynthetic microalgae, a solid medium culture is demanded for the efficient design of biophotovoltaic (BPV) cells. In particular, the conductivity of the culture medium and the contact of microalgae with an electrode are crucial in harvesting electrons in BPV cells. Here, an ion-crosslinked carboxymethylated cellulose nanofiber (CM-CNF)/alginate is proposed as a living hydrogel for the green power generation of Chlorella vulgaris embedded in the hydrogel. The hydrogel crosslinked with Ca2+ and Fe3+ ions showed more efficient BPV properties than the hydrogel crosslinked with only Ca2+ due to the increase of conductivity. The efficient transport of electrons generated by C. vulgaris improves the power generation of BPV cells. Moreover, the fluid channels imprinted in the living hydrogel maintain the viability of C. vulgaris even under the ambient environment by preventing the solid medium from being dried out. [ABSTRACT FROM AUTHOR]