Glass Ionomer Cements (GICs) have found numerous applications as bone fillers, replacements and adhesives, particularly in dentistry due to their tooth like appearance and biocompatibility. GICs are composite materials resulting from the reaction between a polyalkenoate acid and a glass powder (Al2O3-SiO2-CaF2). Unfortunately, use is limited to smaller applications due to their inherent brittleness; weak bridging O-Al-O (polymer-glass) bonds purported to be responsible for material failure. Existing literature describes change in Al-coordination during setting as controlling mechanical properties; as-yet only a speculative extrapolation of existing (unsupported) results. We therefore propose to characterise the micro- and meso-scopic structures of (H and D-labeled) GIC samples, during setting over a clinically-relevant 24 hour period for each sample towards a dynamic structure profile.