Studies regarding the wettability transition of micro- and nano-structured metal surfaces over time are frequently reported, but there seems to be no generally accepted theory that explains this phenomenon. In this paper, we aim to clarify the mechanism underlying the transition of picosecond laser microstructured aluminum surfaces from a superhydrophilic nature to a superhydrophobic one under ambient conditions. The aluminum surface studied exhibited superhydrophilicity immediately after being irradiated by a picosecond laser. However, the contact angles on the surface increased over time, eventually becoming large enough to classify the surface as superhydrophobic. The storage conditions significantly affected this process. When the samples were stored in CO2, O-2 and N-2 atmospheres, the wettability transition was restrained. However, the transition was accelerated in atmosphere that was rich with organic compounds. Moreover, the superhydrophobic surface could recover their original superhydrophilicity by low temperature annealing. A detailed XPS analysis indicated that this wettability transition process was mainly caused by the adsorption of organic compounds from the surrounding atmosphere onto the oxide surface. (C) 2014 Elsevier Inc. All rights reserved.