This study aimed to enhance the compatibility of glass ionomer cement (GIC) with tooth tissue by chemically modifying its primary component, calciumfluoroaluminosilicate (CFAS), through the incorporation of nanorod hydroxyapatite (nHA). The process involved binding L-glutamic acid to nHA, followed by activation and binding of albumin to create nHA immobilized with albumin. This modified nHA was then used to surface-modify CFAS particles, producing nHA-CFAS powder. The modified powder was mixed with poly(acrylic acid) and UV-cured to form GIC containing nHA-CFAS (GIC-nHA). Fourier transform infrared spectroscopy and scanning electron microscopy (SEM) confirmed the successful modification. Cytocompatibility tests with osteoblasts showed that GIC-nHA had superior cell viability and bone formation capabilities compared to the control GIC. The improved histocompatibility is attributed to nHA enhancing the biological activity of osteoblasts, indicating that the surface modification method significantly improves the functional integration of GIC with tooth tissue.