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In this paper, Fe10Co25Ni34Cu23Al8 high-entropy-alloy nanoparticles have been synthesized by the in situ instantaneous electrical wire explosion method. Based on the thermodynamic parameters of the face-centered cubic phase of high-entropy-alloy, the parameters of the five kinds of wires were calculated and controlled, and the stable face-centered cubic structure with good crystallinity was synthesized in one step. The influence of the energy deposition during the electrical explosion on the nanoparticles and their electromagnetic absorption performance was explored. The results show that the face-centered cubic structure high-entropy-alloy with high crystallinity has better electromagnetic wave absorption performance when the energy deposition of the wires is increased. The minimum reflection loss can reach −39.37 dB at 15.34 GHz when the thickness is 1.9 mm and the effective absorption bandwidth is 6.63 GHz. It can provide a strategy for the microstructure and morphology design of high-entropy-alloy nanoparticles in electromagnetic wave absorption and magnetism in the electronics industry. [ABSTRACT FROM AUTHOR]