Targeting next-generation batteries, a multifunctional composite polymer electrolyte (CPE) was developed by integrating glass-fiber-cloth (GFC) with PEO-Li6.4La3Zr1.4Ta0.6O12 (LLZTO). LLZTO improves thermal stability and ionic conductivity. GFC framework further reinforces mechanical strength and facilitates Li-ion dissociation, creating a Li-ion gradient. This synergistic combination presents a promising approach for strategic electrolyte design.