The difference betWeen the systems of CaO-SiO
2-H
2O and CaO-SiO
2-Al(OH)
3-H
2O, was studied,especially the effect of Al
3+ on the crystallinity of tobermorite was focussed. As a result, in the system of CaO-SiO
2-H
2O, tobermorite formed early, howevey, with reaction time forward, tobermorite was replaced by xonotlite. So far as CaO-SiO
2-Al(OH)
3-H
2O was concemed, hydrothermal reaction was carried out under the same condition as CaO-SiO
2-H
2O to study the morphological changes of tobermorite crystals. It was found that Al
3+ accelerated the crystal growth of tobermorite to some extent and was in favor of platy crystals. Moreover, with the Al
3+ content increasing in the starting material, the morphology of tobermorite did not change magnificently, but platy crystals became more and more eminent. As soon as the Al
2O
3 content was over 15.6%, synthetic mineral greatly changed in structure and turned into hibschite different from 1.1 nm tobermorite. Obviously, xonotlite was not apt to form in the presence of Al
3+.