The mesoporous amorphous calcium silicate (MACS) was first synthesized using mesoporous silica SBA-15 as both the template and silicon source, and Ca(NO(3))(2) as the calcium source. The MACS shows a well-defined mesoporous structure with high specific surface area. In vitro bioactivity studies of the MACS were carried out by soaking it in simulated body fluid (SBF) solutions for 4 h up to 5 days. Owing to the high specific surface area and pore volume, the MACS had a significantly enhanced bone-forming bioactivity compared with the conventional amorphous CaSiO(3). The MACS did develop a carbonate-containing hydroxyapatite (HCA) layer on the surface after being immersed in SBF for 4 h with near-spherical agglomerated hydroxyapatite (HA) nanoparticles. At longer soaking times, the number of agglomerated HA particles increased and the surface structure of the samples became more compact. Such MACS could be useful in developing new biomaterials and may have potential use in implanting and drug delivery for tissue regeneration.