Al-MCM-41 mesoporous sieves were synthesized at the ambient temperature by using TEOS as silica source, Al(NO)3 x 9H2O as Al source, and cetyl trimethylammonium bromide as templating agent. The framework and surface structures of the synthesized samples were characterized by XRD, N2-adsorption/desorption isotherms, FTIR and SEM etc. The results showed that the samples were the typical Al-MCM-41 mesoporous sieves with the higher ordered-degree and specific surface area (up to 816 m2 x g(-1)) and the narrower pore diameter distribution. Controlling the highest value of Al/Si with the range of 0.06-0.13, and taking temperature programmed calcination would be beneficial to the formation of the highly ordered Al-MCM-41 mesoporous sieves. The evaluating results showed that the synthesized Al-MCM-41 molecular sieves have a higher catalytic activity for isomerization of endo-tetrahydrodicyclo-pentadiene (endo-TCD) into exo-tetrahydrodicyclo-pentadiene (exo-TCD) and adamantane.