The present work introduces new hybrid material based on the combination of layered double hydroxides (LDH) and a pH-sensitive polymer (PSP), alginate, a polysaccharide widely applied for encapsulating drugs to produce a LDH–polymer nanocomposite, able to act as an effective drug delivery system (DDS) in comparison to the Zn–Al LDH or the polymer alone. Insulin has been chosen as a model drug, being loaded in a Zn–Al LDH matrix. In vitro release profiles were established separately in both the presence and absence of glucose phosphate in pH 7. Drug release studies showed that the in the presence of glucose phosphate release rate increases.