The Langmuir−Blodgett (LB) method has long been used for the preparation of ultrathin films, offering the unique control over the film thickness and the molecular orientation. Here, we report on the deposition and the characterization of LB layers of polyaniline (PANI) nanotubes on solid supports. Stable suspension of the nanotubes in chloroform was obtained by adding sodium dodecyl sulfate (SDS). The nanotubes to SDS ratio is important for the stability of the suspension. Langmuir films were spread at the water/air interface and transferred on gold or ITO glass substrate. The electroactivity of obtained films was investigated using cyclic voltammetry. The degree of assembly of the PANI nanotubes in thin films was characterized by optical microscopy and scanning electron microscopy (SEM). To evaluate the molecular structure and the PANI oxidation state, UV−vis and Raman mapping were used. The PANI nanotube films on the gold support are electroactive with cyclic voltammetry responses closely resembling typical PANI layers. Raman maps reveal that the spatial distributions of SDS and PANI bands are identical, suggesting that only detergent molecules bond to nanotubes are transferred on the support.