Graphene oxide (GO)-polyamidoamine (PAMAM) dendrimer nanocomposite hydrogels were prepared through one-step synthesis by mixing a GO suspension and a PAMAM solution at varying ratio of GO to PAMAM. The materials self-assembled into physically crosslinked networks, mainly driven by electrostatic interactions between the oppositely charged GO nanosheets and PAMAM dendrimer. The chemical structure of PAMAM dendrimer was studied by mass spectrometry, nuclear magnetic resonance spectroscopy and potentiometric titration.The structure and properties of GO-PAMAM nanocomposite hydrogels were investigated by Fourier transform infrared spectroscopy, Raman spectroscopy, X-ray diffraction, scanning electron microscopy and rheometry. The nanocomposite hydrogels exhibited a relatively high mechanical performance with a storage modulus of up to 284 kPa, as well as self-healing property, owing to their reversible and multiple physical cross-links. These hydrogels may be further developed for biomedical applications.2