Compressed fluids such as supercritical CO2 offer marvellous opportunities for the synthesis of polymers, particularly in applications in medicine and dentistry. It has several advantages in comparison to conventional polymerisation solvents, such as enhanced kinetics and simplified solvent removal process. In this study, poly (acrylic acid-co-itaconic acid-co-N-vinylpyrrolidone) (PAA-IA-NVP), a modified glass-ionomer polymer, was synthesised in supercritical CO2 (sc-CO2) and methanol as a co-solvent. The synthesised polymer was characterized by 1H-NMR, Raman and FT-IR spectroscopy and viscometry. The molecular weight of the final product was also measured using static light scattering method. The synthesised polymers were subsequently used in several glass ionomer cement formulations (Fuji II commercial GIC) in which mechanical strength (compressive strength (CS), diametral tensile strength (DTS) and biaxial flexural strength (BFS)) and handling properties (working and setting time) of the resulting cements were evaluated. The polymerisation reaction in sc-CO2/methanol was significantly faster than the corresponding polymerisation reaction in water and the purification procedures were simpler for the former. Furthermore, glass ionomer cement samples made from the terpolymer prepared in sc-CO2/ methanol exhibited higher CS and DTS and comparable BFS compared to the same polymer synthesised in water. The working properties of glass ionomer formulations made in sc-CO2/methanol were comparable and in selected cases better than the values of those made from polymers synthesised in water. © Springer Science+Business Media, LLC 2008.