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There are daily buses from Athens to Mesolongi. The trip takes about 3 and half hours and goes via the cable bridge of Rio-Antirrio. Buses from Athens depart from Kifissos KTEL Bus Station (Bus 051 Omonoia-Kifissos and Bus X93 Athens Airport-Kifissos).
There are also buses to Mesolongi from other towns of Greece, including Patras, Ioannina, and Thessaloniki. Bus schedules from other Greek towns may not be daily but twice or three times a week.
To go from Athens to Mesolongi by car, you take the National Highway Athens-Patras. After you cross the cable bridge of Rio-Antirio, you follow the signs to Mesolongi.