The magnetic properties of highly grain-oriented electrical steel vary along different directions. In order to investigate these properties, standard Epstein samples were cut at different angles to the rolling direction. The hard magnetization direction was found at an angle of 60° to the rolling direction. To compare the measured and fitting curves, when the magnetic field intensity is higher than 7000 A/m, it is appropriate to simulate the relation of magnetic permeability and magnetization angle using the conventional elliptical model. When the magnetic field intensity is less than 3000 A/m, parabolic fitting models should be used; but when the magnetic field intensity is between 3000 and 7000 A/m, hybrid models with high accuracy, as proposed in this paper, should be applied. Piecewise relation models of magnetic permeability and magnetization angle are significant for improving the accuracy of electromagnetic engineering calculations of electrical steel, and these new models could be applied in further industrial applications.