This research aimed to modify the Nias' cacao pod husk cellulose by using Microwave-assisted Organic Synthesis (MAOS) method to produce carboxymethyl cellulose and its application as lithium-ion batteries' biopolymer electrolyte membrane. There were two main stages of modification of Nias' cacao pod husk cellulose i. e. cellulose alkalization and cellulose carboxymethylation process (etherification stage). Lithium-ion batteries' biopolymer electrolyte membrane was fabricated through the casting solution technique, where the blend of Methylcellulose/Carboxymethyl cellulose (MC/CMC) (80/20) (w/w) was complexed to 10 % (w/w) of lithium perchlorate. The determinations of functional groups, molec-ular structure, crystallinities, and thermal stability were conducted using Fourier Transform Infrared, Nuclear Magnetic Resonance, X-Ray Diffraction, and Thermogravimetry Analysis, respectively. The lithium-ion biopolymer electrolyte of the 10 % lithium perchlorate-complexed MC/CMC (80/20) blend shows ionic conductivity, tensile strength/elongation at break, thermal stability are 5.91 × 10 À 3 S cm À 1 , 30.69 MPa/31.83 %, and 279.40-341.05 °C. Based on the results, the prepared biopolymer electrolyte of 10 % lithium perchlorate-complexed MC/CMC (80/20) fulfills the separator (solid electrolyte) requirement for lithium-ion battery application.