Pb0.7Sr0.3TiO3/La0.7Sr0.3MnO3 (PST/LSMO) thin film has been deposited on Si substrate by chemical solution deposition. Obvious changes in dielectric constant and loss as functions of frequency and magnetic field were observed in PST/LSMO thin film. By applying both dc bias electric and magnetic fields, apparent dielectric anomalies were observed in the “butterfly-hysteresis” curves. These effects may be useful for practical application. The mechanism for the magnetocapacitance effects in PST/LSMO is rationalized by combining the Maxwell–Wagner capacitor model and the magnetoresistivity and magnetostriction of the LSMO.