A structural study of glass-ionomer cement (GIC) dental restoratives has been completed. Transmission electron microscopy, selected area electron diffraction, and X-ray diffraction studies indicate domain-like microstructure in a new experimental material, whereas a featureless amorphous gel-like microstructure exists in the conventional GIC. Nuclear magnetic resonance studies were also conducted. The new experimental GIC contains domains of (i) bonelike material (apatite), (ii) mesoporous material and (iii) other framework structures (aluminium phosphate in the high cristobalite structure), with its setting chemistry a restructuring of the aluminosilicate glass around the template of poly(acrylic acid). Conventional glass-ionomer cement may set by a similar but slower process. Leaching properties of glass-ionomer cements are also explained.