The deposition of polypyrrole (PPy) on a Ti surface is commonly employed to enhance the material’s properties for different applications such as supercapacitors, biomedicine, and corrosion resistance. Instead of complex or costly polymerization procedures for the PPy synthesis on the Ti metal surface, we utilized the effect of a simple and inexpensive laser ablation of the Ti surface in the open-air environment to prepare a hydrophilic TiO2 surface. In this condition, a thin PPy layer with remarkable nanostructures such as nanorings (∼80 nm) and nanotubes (∼245 nm) was deposited on a selective and desired pattern of ablated Ti areas through the chemical vapor deposition process using ferric chloride (FeCl3) solution as a pyrrole oxidizer. Raman and X-ray photoelectron spectroscopy (XPS) analyses confirmed the PPy formation on the Ti surface. The creation of these nanostructures was due to the micro/nanomorphology of the ablated Ti substrate. Water contact angle (WCA) measurements indicated the hydrophobic behavior of the PPy/Ti surface by the aging effect after 24 weeks with the change of WCA from 20° to 116°. The change in the surface chemical composition upon adsorption of airborne organic compounds with the long-term storage of PPy/Ti surface in air was studied by the XPS test.