Spyridōn-Alkibiadīs Zambelios was born on the Ionian island of Lefkas in 1815. His father Iōannīs, trained in law, was a member of the Filikī Etereia and author of patriotic theatre plays (“historical tragedies”, as he termed them).

Spyridōn attended the Lefkas lyceum and in 1833 enrolled in the Ionian Academy of Corfu, where he was taught by Andreas Moustoxydīs (1785–1860), one of the founding fathers of Greek historiography. He then continued his studies in Bologna and Pisa and travelled to several European cities, where he first came into contact with the texts and the archival material on the basis of which he shaped his historiographical views. From the age of 17 he had also started to write poetry.

After his return to the Ionian Islands he worked as a journalist; in 1850 he was elected member of the assembly of the Ionian Islands (Īnomenon Kratos tōn Ioniōn Nīsōn), which voted for union with the Greek state; its suppression by the British authorities in the following year brought Zambelios’ brief political career to an end and marked the beginning of his turn to history-writing.

In 1852 Zambelios published, in Corfu, the Asmata dīmotika tīs Ellados: Ekdothenta meta meletīs istorikīs peri mesaiōnikou ellīnismou (“Folk songs of Greece: Published with a historical study on medieval Hellenism”). This was followed five years later by his other major work, the Byzantinai Meletai: Peri pīgōn tīs neoellīnikīs ethnotītos apo Ī’achri I’Ekatontaetīridos (“Byzantine studies: On the origins of the modern Greek nationality from the 8th until the 10th century”, 1857).

His work addresses various fields: philology and the history of the Greek language; the historical novel; editions of historical sources; and history-writing. To the first category belong some articles he published in the journal Pandōra between 1856 and 1860, and the 1889 publication Pothen ī koinī lexis Tragoudō? Skepseis peri ellīnikīs poiīseōs (“Whence the common word tragoudō, to sing? Thoughts on Greek poetry”, 1889; on the work of Dionysios Solōmos). As regards the second category; Zambelios wrote two historical novels set in Crete under Venetian rule: Istorika Skīnografīmata (“Historical scenes”, 1860) and Krītikoi Gamoi (“The Cretan weddings”, Turin 1871). The third category includes his Italoellīnika, ītoi Kritikī pragmateia peri tōn en tois archeiois Neapoleōs anekdotōn pergamīnōn (“Italian-Greek texts: A critical treatise on the unpublished parchments in the archives of Naples”, 1864), an edition of 10th- to 14th-century documents in the dialect of the Greek population of southern Italy. However, Zambelios’s main claim to fame rests on his historical writings, which, apart from his two major works, include several articles in Athenian periodicals such as Pandōra and the Spectateur de l’Orient.

Zambelios’s history-writing follows the French Romantic school, and aims to rebut the negative representation of the Byzantine Middle Ages established by Montesquieu, Voltaire, and Gibbon. Zambelios put forward his critique of what he saw as a blinkered denigration in the extremely lengthy introduction to his Dīmotika Asmata, highlighting instead the slow, but continuous Hellenization of the Eastern Roman Empire. His procedure was indebted to Augustin Thierry’s principle that, since the history of a subjugated people is not documented in official archival records, its history must be reconstructed from whatever manifestations of its “popular spirit” have come down to us. Zambelios accordingly writes Byzantine history as that of a subjugated people – the Greeks – gradually taking control of their conquerors’ (“Roman”) empire. The resulting Hegelian synthesis is the Byzantine Empire. As Zambelios himself acknowledged, this Greek-centred view of the past had to rely substantially on “unofficial” historical sources such as the demotic songs of the modern Greeks. It thus also established, retroactively, a cultural continuity between Byzantium and modern Greece.

Zambelios moved to Livorno in 1870 and died in 1881 in Zug, Switzerland.