We investigated the effect of various aluminum sources on the morphology and microstructure of nanoporous Al-SBA-15. With aluminum tri-sec-butoxide (Al-TSB), very large, ordered hexagonal rods of Al-SBA-15 covered by nanostairs and terraces were synthesized. Such a morphology was not obtained with an inorganic Al source (sodium aluminate) or with organic sources seemingly similar to Al-TSB, such as aluminum tri-tert-butoxide, aluminum tri-n-butoxide, or aluminum isopropoxide. The results obtained from X-ray diffraction, scanning electron microscopy/transmission electron microscopy, N-2 adsorption/ desorption, and high-performance Xe-129 NMR suggest that preparing an organic Al-Si precursor by premixing liquid organic Al and Si sources (Al-TSB and tetraethyl orthosilicate) is crucial in obtaining highly ordered mesoporous Al-SBA-15 materials with a well-defined morphology.