In this study, to investigate the effect of volume concentration on core loss in the high frequency band (~MHz), easy-plane soft magnetic composites (SMCs) of FeSiAl particles with different volume concentrations were prepared successfully by magnetic field orientation. The permeability of the SMCs was decomposed into the domain wall component and the spin component and was well simulated. The core loss was successfully decomposed into hysteresis loss, eddy current loss and excess loss. It was shown that the permeability of the SMCs was continuously improved as the volume concentration of FeSiAl in the SMCs increased, while the core loss decreased first and then increased due to the different performances of the hysteresis loss, eddy current loss, and excess loss. Samples with a permeability of 310 exhibited the lowest core loss of 399 kW/m3 (f=3 MHz, 10 mT). The results indicated that there is an optimal volume concentration at which SMCs have a relatively high permeability and minimum core loss.