With the emerging power electronic technologies, numerous electrical devices use high-frequency and nonsinusoidal supplies. Such sources generate complex harmonic fields that overburden the accurate prediction of core losses using the conventional finite element method (FEM). Thereby, to predict core losses under those high-frequency and nonsinusoidal supplies accurately, this study first built a test system for core losses measurement of ferromagnetic materials (e.g., soft ferrite, laminated steels, and nanocrystalline alloy) fed by the square and pulsewidth modulated (PWM) supplies. Then, the loss prediction problems of the classical core loss model under high-frequency and nonsinusoidal supplies are revealed. Afterward, an improved FEM-based core loss model is proposed, which includes a piecewise variable parameters based hysteresis loss model, an eddy current loss model considering different cross sections of magnetic circuit and supply waveforms, and improved excess loss coefficients. Experimental validations on different materials, the nanocrystalline alloy in an 11-kVA intermediate frequency transformer, the ultrathin silicon sheets in a 10-kW high-speed permanent magnet motor, and the nanocrystalline alloy in a 3-kW wireless power transfer system, are conducted systematically. The effectiveness and generality of the improved core loss model were verified.