Herein, the work describes a comparative study of the magnetocaloric performance along different magnetization directions of cluster Gd‐based fibers for potential applications. Experimental results indicate that there exists the relatively obvious difference of magnetocaloric effect (MCE) in both longitudinal and transverse magnetization directions. Moreover, the isothermal magnetic entropy changes −ΔSm of 10.62 J kg−1 K−1 and refrigerant capacity (RC) of 756.37 J kg−1 of cluster fibers in transverse direction exhibit a higher value than those in longitudinal direction at relatively high field. This distinction depends on magnetic coupling (magnetic charges induced by electron spin‐orbit polarization) among cluster fibers and magnetic anisotropy (namely magnetic moment rotation) by the action of high magnetic field energy. Therefore, the cluster fibers by changing magnetization direction can provide an effective MCE modulation or to be a candidate for practical magnetic refrigeration applications.
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