In this study, we successfully grafted chitosan (CS) onto multi-walled carbon nanotubes (MWCNTs) to enhance their properties and potential applications in the biomedical field. FTIR spectroscopy confirmed the successful covalent bonding of CS onto MWCNTs, indicated by the new absorption peak of the amide bond (–CONH–). Thermal analysis showed that the modified MWCNTs (MWCNT-CS) had significant weight loss around 260 °C, suggesting the decomposition of hydroxypropyl chitosan, and confirming its presence in the nanocomposite. SEM images revealed that CS grafting improved the dispersibility of MWCNTs, a property crucial for their use as nanofillers in polymers. Moreover, the micro-tensile bond strength of dentin surface increased with increasing MWCNT-CS concentrations, indicating the potential of MWCNT-CS as a pretreatment for dentin bonding. After simulated aging, the bond strength remained significantly higher for MWCNT-CS groups compared to those without pretreatment. In biocompatibility assessment using the MTT assay, MWCNT-CS showed higher cell viability than MWCNT, suggesting improved biocompatibility after CS modification. The results of this study suggest that CS-modified MWCNTs could be promising materials for applications in dentin bonding, dentin mineralization, bone scaffolding, implants, and drug delivery systems.