Developing biopackaging materials is a key for environmental, social, and economic sustainability. Herein, a newly designed gelatin composite film was prepared by incorporating biomass-derived aldehyde (BDA) and aminated graphene oxide (AGO), denoted as GBAF. FTIR, XPS, and primary amino group content tests demonstrated the successful preparation of AGO with different amino group contents. FTIR, XRD, and SEM analyses of GBAFs indicated strong interactions among AGO, BDA, and gelatin as well as the uniform dispersion of AGO in the film matrix. TG-DSC analysis showed that the GBAFs had higher thermal stability, and introducing AGO helped to improve the thermal stability of the GBAFs. WVP and gas permeability tests showed that the addition of AGO and BDA into the gelatin film reduced the transmission rate of water vapor, O 2 , and CO 2 , respectively. Additionally, the GBAF prepared from AGO with the highest primary amino content had the best tensile strength (2.45 MPa) due to the rigidity of AGO and covalent cross-linking between gelatin and BDA. Its tensile strength was much higher than that of the composite film without AGO (1.36 MPa) or BDA (1.59 MPa). Owing to its environmental friendliness, low toxicity, and sustainability, the as-prepared GBAF shows the potential to be used in sustainable biopackaging.