Founded in 1834, the Archaeological Museum of Syros is one of the oldest museums in Greece. It was housed for a short time in the High School and then in a building on today's Nisaki. Since 1899, it has been operating in four rooms of the Ermoupolis town hall. Initially, it included in its exhibition objects from various areas of the Cyclades, as well as the archaeological collection of I. Kokkonis, which consisted mainly of marble inscriptions found on the island. In 1898, C. Tsountas carried out excavations in the Early Cycladic settlement of Kastri and at the cemetery of Chalandriani. The local government and the citizens of Syros all demanded that the antiquities remain on the island, resulting in the allocation of four rooms of the Neoclassical town hall of Ermoupolis by the then mayor, St. Vafiadakis. The rooms were designed, in accordance with the specifications of the time, by the municipal architect D. Eleftheriadis. Tsountas himself transferred in 1901 finds from the excavations of Chalandriani from the National Archaeological Museum to the new Museum. Thus, the Archaeological Museum of Syros first opened at a time when the capital of the island had all the characteristics of a developed European city. The town hall of Ermoupolis itself was constructed in 1876 under the supervision of E. Ziller.

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