Although hydrogel electrolytes have attracted considerable attentions due to high water retention and low leakage, their vulnerability and low conductivity still pose challenges in large-scale applications. In this work, a mechanically strong and highly conductive poly (acrylic acid) (PAA) electrolyte reinforced by cellulose nanofibrils (CNFs) is developed via versatile blending followed by polymerization. As a result of physical entanglement and hydrogen bonding, the mechanical strength of the PAA electrolyte is enhanced from 0.656 to 1.875 MPa at a CNF loading of 3 wt%, and the dimensional swelling is suppressed to half of its original level. The ionic conductivity of the composite electrolyte is improved by 100% due to excellent ion-transfer paths created by the hydroxyl groups exposed on the surfaces of CNFs. Furthermore, the CNF/PAAs exhibit preferable elasticity and flexibility with the maximum elongation at break reaching greater than 600%. These electrolytes are able to maintain the initial ionic conductivity even after being stretched to 100% elongation for 500 circles. After assembling with an air cathode and an aluminum anode, the as-prepared Al−air battery show good discharging performance, demonstrating promises for applications in portable and flexible electronic devices.