A new class of activated mesoporous Al-MCM-41 layers was deposited on Fe-CrAl metallic foils in the presence of cationic surfactant cetyltrimethylammonium bromide under basic conditions by an in-situ hydrothermal method. The characterization techniques including X-ray dif-fraction, nitrogen adsorption and transmission electron microscopy, as well as field-emission scanning electron microscopy were performed to investigate the pore structure and surface morphology of the Al-MCM-41 layers. The Al-MCM-41 materials are of amorphous structure but exhibit large BET surface area (up to 757.0 m2/g) and pore volume (up to 0.72 cm3/g), as well as a mean pore diameter of 3 nm. The layers deposited on the FeCrAl foils are continuous despite with a few of holes on the sur-face.