The surface contact angles of aluminum-based materials is regulated and controlled by using femtosecond laser pulses with different energies, and the transformation mechanism of wettability is analyzed and studied. The results show that the final stable wettability state of aluminum-based material surfaces after the femtosecond laser processing and aging treatment is related to the laser energy and the aging time. With the increase of the laser energy, the surface contact angle is changed from 70° to above 150°. The morphology, roughness and chemical compositions of aluminum-based surfaces are studied under different pulse energy processing conditions. The results show that the wettability of a laser-processed sample changes from a hydrophilic state to a final super-hydrophobic state. The super-hydrophobic surfaces can be obtained in different pulse energy regions, but there are non-periodic or periodic structural differences in their surface microstructures, and the formation mechanisms of hydrophobic properties are different.