A novel polyaniline (PANI)/H2Ti4O9 lamellar nanocomposite has been synthesized by in situ polymerization using aniline intercalation Compound (ANT)/H2Ti4O9 as the intermediate. According to the experimental results, the ANI within the inter-layer spacing of the layered H2Ti4O9 material may be oriented in a single-layer arrangement, with the benzene rings perpendicular to the layer sheets. After polymerization, a monolayer of PANI chains within the confined galleries was produced. The PANI/H2Ti4O9 nanocomposite has been Studied by electrochemical methods, which revealed good redox activity.