The invention discloses a preparation method of a single-phase multiferroic thin film. The preparation method comprises the steps that after a substrate is cleaned, a target material and the substrateare put into a coating cavity, and the pressure intensity in the cavity is adjusted; the temperature of the substrate is increased, then the cavity is filled with O2, and the pressure intensity in the cavity is adjusted; the distance between the substrate and the target material is adjusted, and the substrate and the target material are adjusted to rotate; the repetition frequency and pulse energy of a laser are adjusted; thin film deposition is conducted, and then heat preservation is conducted; and after heat preservation, cooling is conducted to the room temperature. The chemical composition of the target material is (1-m)BiTi(1-n) / 2FenMg(1-n) / 2O3-mCaTiO3, wherein 0<m<1, and 0<n<1. The preparation method provided by the invention has unique advantages when a thin film containing complex oxide is prepared, and the growth of the thin film can be precisely controlled in the preparation process. The invention further provides the single-phase multiferroic thin film and the applicationof the single-phase multiferroic thin film in an electronic device. The prepared thin film is compact and uniform, has ferroelectricity, ferromagnetism and magnetoelectric mutual controllability at the same time under room temperature, can be used in the electronic device containing a thin film, and has wide application prospects.