In this study, CNCs were used to improve the adhesion performance of PVA/CNC electrospun membranes onconcrete surfaces. The PVA/CNC 5% (CNC content is 5 wt% based on PVA weight) was prepared byconventional electrospinning. Light microscope, scanning electron microscope (SEM), and bonding test(shear/tensile) were utilized to evaluate the morphology and adhesion properties of the PVA/CNC electrospunmembrane. The results showed that the addition of CNCs made some changes in the morphology of thePVA/CNC membrane. Interestingly, the adhesion strength of PVA/CNC membrane on concrete surfaces hasbeen significantly increased by 102.3 % compared to that of PVA membrane. For the PVA membrane case,the bonding failure occurred in the adhesion zone (areas between membrane and concrete). By contrast, thebreak in the cohesion zone (inside membrane) was observed for PVA/CNC membrane case. These resultssuggest the potential use of PVA/CNC membrane as a green solid adhesive on concrete surfaces.