Island-like structure induced by hydroxyl groups has been demonstrated to pose significant influence on tuning surface morphology and wettability. Herein, with an intention to better understand this structural transformation, hydroxyl groups both from nanoparticles and substrates were controlled during the thermally-driven deposition procedure. The results show that hydroxyl groups originated from nanoparticles facilitate the fabrication of island-like structure, while these groups from substrates confine. Representatively, hydroxyl-rich TiO2 n...