Hydrotalcite-type materials, or layered double hydroxide (LDH), are very promising in applying slow-release drug systems through ion exchange and delamination characteristics at acidic pH. In this paper, Zn/Al LDHs in 2:1 and 3:1 molar ratios intercalated with the drug ibuprofen (IBU) were added to chitosan/alginate membranes. In the release tests, an increase in the solubility of the drug in the membranes could be observed, and the percentage of drug release is lower than the percentage of drug release in the free samples. The following release percentages were obtained: 15.48% and 17.5% of the drug in water, and 23.22% and 26.25% of the drug in PBS buffer solution, respectively, for membrane samples containing Zn 2 Al-IBU and Zn 3 Al-IBU LDHs. Thus, the synthesized hybrid membranes (chitosan/alginate-LDH-IBU) are promising in the application as resorbable membranes for bone grafting with drug release.