The invention discloses a tetranuclear dysprosium cluster compound based on 2-formyl-8-hydroxyquinolinetrihydroxyaminomethane Schiff base as well as synthesis methods and application thereof. The chemical formula of the tetranuclear dysprosium cluster compound is as follows: [Dy4(Cl4H14N2O4)4(CH3COO)4(CH3OH)2].2H2O and the tetranuclear dysprosium cluster compound belongs to a trigonal crystal system and has an R-3 space group. The invention provides two methods for synthesizing the tetranuclear dysprosium cluster compound; the methods are simple and have relatively high yield and good repeatability. The applicant researches and finds out that the cluster compound has a single molecular magnet behavior and can be used for preparing magnetic materials.