The invention discloses a preparation method of a crosslinked bionic coating layer with two formyl-and-amino-containing phosphorylcholine polymers. The method comprises the following steps: polymerizing a phosphorylcholine hydrophile group-contained vinyl monomer with a formyl-containing vinyl monomer or an amino-contained vinyl monomer through a simple solution free radical to synthesize the twoformyl-and-amino-containing phosphorylcholine polymers, dissolving the two formyl-and-amino-contained phosphorylcholine polymers in a polar solvent, coating the surface of a material to be modified with the two formyl-and-amino-contained phosphorylcholine polymers, drying the surface in air, and then heating the material in distilled water, so as to prepare the crosslinked bionic coating layer with a cell cover film imitated structure. The method is easy for preparation and convenient to operate; a new way is provided for obtaining the crosslinked bionic coating layer with excellent blood compatibility. The modified material which is of the cell cover film imitated structure has a wide application prospect in the fields of blood purification, in-vivo material implantation, tissue engineering, drug controlled release, biosensors and the like.