The invention discloses a preparation method of a carbon-dioxide-base polyurea high polymer material, belonging to the technical field of preparation of high polymer materials. The method solves the problem that the carbon-dioxide-base polyurea in the prior art can not satisfy the requirements, and widens the application range of the carbon-dioxide-base polyurea. The preparation method comprises the following step: polymerizing amino-terminated polyurea oligomer with a chain extender, an epoxy resin, an alkyd resin, a phenol formaldehyde resin, a urea-formaldehyde resin or other active-terminated oligomers to obtain the carbon-dioxide-base polyurea high polymer material. The structural formula of the amino-terminated polyurea oligomer is disclosed as Formula I. The preparation method is green and environment-friendly, has the advantages of no pollution, simple technique, favorable atomic economical efficiency and wide application range, can prepare high polymer materials with various properties through further reaction between amino-terminated polyurea oligomers with different structures and different substrates, and is suitable for multiple purposes.