In this study, the effects of drying temperature and mechanical pressure on the surface structure and dynamical properties of polyaniline (PAni) were studied. PAni was synthesized through the aniline polymerization process in the presence of ammonium persulfate in acidic medium and normal methyl-2-pyrrolidine solution. The obtained solution was dipped on a substrate of quartz glass. Atomic force microscopy (AFM) analysis based on nano-indentation tests were used to determine the values of hardness, Young’s modulus and Poisson’s ratio of the films. The results of the analysis of the scanning electron microscope demonstrated that the surface morphology of the film is changed from a fiber-to-interconnected cross-linked networkby increasing the drying temperature. The transmission electron microscope analysis showed that the diameter of the fibers on the surfaces dried at 318 K and 418 K was 18 and 30 nm, respectively. AFM results showed that the mean surface roughness of PAni film at 318 K without mechanical pressure was 63 nm, while for the film pressed at 5 MPa was less than 35 nm. Thermo-mechanical analysis showed that the glass transition temperature of the PAni film prepared without mechanical pressure and the film pressed at 5 MPa were 386 K and 378 K, respectively. Investigating the temperature dependence and applied pressure on the film surface in determining the viscoelastic properties of the PAni nanostructured film can provide readers with appropriate information about the storage and loss modulus of the film and the activation energy of the polymer layer during the thermal decomposition process.