The paper focuses on the obtaining of novel nanocomposite hydrogels based on polyacrylamide and layered double hydroxides (LDHs) modified with double bonds. The modification of LDH clay was investigated by FTIR, X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) analyses. Mechanical properties of the nanocomposite hydrogels were employed by compression and rheological measurements. The formation of exfoliated and intercalated structures was evidenced in transmission electron microscopy (TEM). Chemical cross-linking of hydrogels using both classical cross-linker and modified clay was an efficient method to improve the mechanical properties of novel nanocomposite hydrogels. These hydrogels with improved mechanical properties could be further tested for biomedical applications such as tissue engineering.