Under hydrothermal condition, kenaf cellulose carbamate (KCC) was synthesized using urea and kenaf core pulp (KCP) without catalyst and organic solvent. The KCC was prepared with various urea/KCP ratios (2:1, to 4:1 and 6:1) with the aid of autoclave and oil bath, whereas the regenerated KCC membranes were formed via solution casting method. The physical and thermal properties of KCC were studied. The urea/KCP ratio used in preparing KCC corresponds with the nitrogen percentage obtained in KCC. The formation of the regenerated KCC membranes could be confirmed by the existence of cellulose II through X-ray diffraction (XRD) study. As examined by Field emission scanning electron microscope (FESEM), the regenerated KCC membranes possessed the greater pore size structures at higher urea concentration. Mechanical results showed the tensile strength and modulus of regenerated KCC membranes have improved up to 43.4% and 76.9%, respectively, as compared to native KCP membrane. It can be concluded from the findings that synthesizing KCC and its membranes with improved mechanical properties has broad prospects for potential industrial applications such as biomembranes and packaging materials.