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Solid oxide cells (SOCs) are attracting much more attention as promising energy conversion and storage devices. One of the challenges of optimizing of solid-oxide cells’ performance is that there are not enough triple-phase boundaries (TPB) in the electrode bulk. To enhance the reaction area for SOCs, Sr₂Fe_1.5Mo_0.5O_6-δ nanofibers are synthesized by electrospinning with metal nitrate precursors and used for SOC electrodes operated in both humidified air and a hydrogen atmosphere. SFMO nanofibers display a highly porous and crystallized perovskite structure and continuous pathways by XRD analysis and SEM observation. The average diameter of the SFMO nanofibers after sintering is about 100 nm. The La_0.8Sr_0.2Ga_0.8Mg_0.2O_3-δ(LSGM) electrolyte-supported symmetrical cell with the SFMO nanofiber electrode exhibits enhanced electrochemical performance in humidified air and an H₂ atmosphere. Moreover, a distribution of the relaxation time method is used to analyze the impedance spectra, and the polarization peaks observed are assigned to correspond different electrochemical processes. The results indicate that the SFMO nanofiber with an improved nanostructure can be the potential material for the SOC electrode.