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Intranasal route, ensuring suitable bioavailability of medicines under circumvention of the gastrointestinal degradation and hepatic first-pass elimination, has been a popular choice for drug delivery. Among nasal dosage forms, mucoadhesive solid inserts have been shown to resist mucociliary clearance and provide a prolonged nasal residence time. Hence, the purpose of this study was the preparation and characterization of nasal inserts composing of polyelectrolyte complexes (PECs) based on k-carrageenan (k-CA) and chitosan (CS) to boost therapeutic efficacy of sumatriptan succinate in the treatment of migraine headache. k-CA/CS PECs were developed in different molar ratios, subjected to lyophilization in small inserts in the presence of sumatriptan succinate, and finally investigated for water uptake ability, mucoadhesive potential, and drug release profile. The formation of PEC between the two polymers was affirmed by Fourier transform infrared spectroscopy (FTIR). Based on the results, it was revealed that the polyanion/polycation molar ratio plays a critical role in modulating the characteristics of the inserts, and among all the formulations, the one comprising k-CA/CS PEC with molar ratio of (4:1), (k-CA/CS (4:1)), demonstrated the highest water uptake ability and mucoadhesive potential and provided a more controlled release of sumatriptan succinate. This study illustrates the potential of the lyophilized inserts based on the k-CA/CS PECs, especially k-CA/CS (4:1), for efficient delivery of sumatriptan succinate via the nasal route of administration and suggests a potential therapeutic approach for the termination of migraine attacks.