To develop a material with potential biomedical applications, novel gelatin films were prepared by cold-casting method using cerium(III) and genipin solution as cross-linking agents, and surface modified with dendritic molecules. The structure and properties of the synthesized gelatin films were investigated by ATR-FTIR, mechanical tests, swelling behavior and water vapor permeability (WVP). The results showed that cross-linking could improve the mechanical and microbiological properties and lower the hydrophilic property of gelatin films. According to ATR-FTIR analysis, it can be concluded that the dendronization took place on only one of the faces of the films. The results have shown that the experimental methodology performed allows one-surface modification, so a novel biomaterial was obtained in the form of a film with good properties and dendritic structure in one face (hydrophobic and hydrophilic faces), rendering a multivalent structure useful in biomedicine development.