abstract
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Composite poly(vinylidene fluoride) (PVDF) aerogels were synthesized via crystallization-induced gelation in DMF/ethanol mixtures with hydroxylated carbon nanotubes (CNT-OH) as nanofillers. The interplay between solvent composition and CNT-OH content was found to control gelation and the development of crystalline phases. FTIR analyses showed that CNT-OH selectively promotes the electroactive ß and ¿ phases, up to 14% and 66%, respectively, while inhibiting the non-polar ¿ phase to 31%. Adding H
2 O as a secondary non-solvent further stabilized the ß/¿ phases while completely inhibiting the ¿ phase, as well as promoting notable morphological changes. Additionally, aerogels with CNT-OH 1 wt% provided the best mechanical improvement and also influenced vibrational characteristics, causing concentration-dependent shifts in the ß-phase band that indicate strong interfacial interaction. These findings demonstrate that CNT-OH-assisted crystallization-induced gelation can produce PVDF aerogels with customizable polymorphism and improved mechanical properties for advanced multifunctional applications. © The Author(s), under exclusive licence to The Materials Research Society 2025.