We have developed a high-strength light-cured glass-ionomer cement (LCGIC). The polymer in the cement was composed of the 6-arm star-shape poly(acrylic acid) (PAA), which was synthesized using atom-transfer radical polymerization. The polymer was used to formulate with water and Fuji II LC filler to form LCGIC. Compressive strength (CS) was used as a screening tool for evaluation. Commercial glass-ionomer cement Fuji II LC was used as control. The results show that the 6-arm PAA polymer exhibited a lower viscosity in water as compared to its linear counterpart that was synthesized via conventional free-radical polymerization. This new LCGIC system was 48% in CS, 77% in diametral tensile strength, 95% in flexural strength and 59% in fracture toughness higher but 93.6% in shrinkage lower than Fuji II LC. An increasing polymer content significantly increased CS, whereas an increasing glass filler content increased neither yield strength nor ultimate CS except for modulus. During aging, the experimental cement showed a significant and continuous increase in yield strength, modulus and ultimate CS, but Fuji II LC only showed a significant increase in strength within 24 h. The experimental cement was very biocompatible in vivo to bone and showed little in vitro cytotoxicity. It appears that this novel LCGIC cement will be a better dental restorative because it demonstrated significantly improved mechanical strengths and better in vitro and in vivo biocompatibilities as compared to the current commercial LCGIC system.