Glucosyltransferase (GTF) is a key enzyme in biofilm formation of Streptococcus mutans, the primary driver of dental caries worldwide. The identification of potential new GTF inhibitors may contribute to combating this disease and devising new treatments for it. This study is a component of a virtual screening strategy. The main objective was to identify natural compounds that can effectively inhibit this enzyme. To achieve this, we used a library of 545 molecules derived from medicinal and aromatic plants of Morocco, available in the Moroccan Plant Database (MPDB). PyRx software was used for molecular docking simulations, while 3D protein modeling and visualization were performed using PyMOL software. Molecular interactions were analyzed using Discovery Studio. The selected ligands were further evaluated for their ADME properties via the SwissADME server. Finally, molecular dynamics simulations were performed using GROMACS under a Linux environment to study the stability of the complexes formed. Docking results showed that cupressuflavone (Tetraclinis articulata) and (-)-catechin gallate (Arbutus unedo) are the best potential GTF inhibitors, with affinities of -9.1 and -8.8 kcal/mol, respectively. Molecular interaction analysis showed a robust interaction network with both phytocompounds and GTF. The analysis of ADME properties indicated that (-)-catechin gallate and cupressuflavone exhibit favorable pharmacokinetic properties. In conclusion, cupressuflavone and (-)-catechin gallate have been identified as promising inhibitors of glucosyltransferase, offering potential leads for new therapeutic strategies against dental caries.