ABSTRACT: In this study, two nitrile-functionalized spiro-twisted benzoxazine monomers, namely 2,2'-((6,6,6',6'-tetramethyl-6,6',7,7'-tetrahydro-2H,2'H-8,8'-spirobi[indeno[5,6-e][1,3]oxazin]-3,3'(4H,4'H)-diyl)bis(4,1-phenylene))diacetonitrile (TSBZBC) and 4,4'-(6,6,6',6'-tetramethyl-6,6',7,7'-tetrahydro-2H,2'H-8,8'-spirobi[indeno[5,6-e][1,3]oxazin]-3,3'(4H,4'H)-diyl)dibenzonitrile (TSBZBN) were successfully developed as cross-linkable precursors. In addition, the incorporation of the nitrile group by covalent bonding onto the crosslinked spiro-twisted molecular chains improve the miscibility of SPE membranes with lithium salts while maintaining good mechanical properties. Owing to the presence of a high fractional free volume of spiro-twisted matrix, the -CN groups would have more space for rotation