Weekly Georgian Etymology: ბერძენი berdzeni 'Greek person', from Old Georgian ႡႤႰႻႤႬႨ berdzeni, perhaps via Megrelian or Abkhaz, from Greek Βυζάντιον, archaic city-state and later capital of the Roman Empire. Like other words for Greeks, it stems from a specific subset of Greeks.
It is often attested in early works specifically in the context of Byzantine-Muslim conflicts, such as the 9th c polemical iconophile Martyrdom of Konstantin-Kakha: განამტკიცა ღუაწლი ბერძენთაჲ და მრავალნი ჭალაკნი აღაშჱნნა, რომელნი მოოჴრებულ იყვნეს აგარიანთა მიერ.
Which translates: "He strengthened the forces of the Byzantines and built up the islands which had been laid waste by the sons of Hagar [= Arabs]"
More pointedly, in Old Georgian ბერძენი Berdzeni is used in contrast to an older Georgian word for Greek, იონი Ioni 'Ionian'. This reflects the common fact that words for Greeks in different languages usually come from specific tribes or subsets of Greeks, not Greeks as a whole.
Thus Homer refers to Danaans, Argives and Akhaians, a name that shows up in Hittite texts as Aḫḫiyawa. Other lgs used other tribes' names:

Ionia: Old Armenian յոյն yoyn, Aramaic ܝܘܢ yawān, Arabic يوناني yūnāniyy
Boeotian Graia: Latin Graecus etc
Selloi: Greek Ἕλλην
This further reflects the fact that 'Greece', as a unified concept referring to more than a shared language and culture, did not exist in antiquity. Thus it is not surprising that Kartvelian would have used at least two separate roots to refer to Greek peoples.
It seems likely that both ბერძენი Berdzeni and იონი Ioni are extremely early borrowings. Greek settlement in the eastern Black Sea region began at least by the first half of the first millennium BC in colonies like Bathys Limen (> Batumi) and Dioskourias (> today's Sukhumi).
It also seems likely that Byzantion played an important role in this, sitting astride the important Bosporus trade routes. It was founded according to tradition in 657 BC as a colony of Megara, and by the time Constantine refounded it as his capital, it was about 1000 years old.
For the rest of the Greek world, Byzantion did not loom large until it became the capital of a world empire, but for the almost the entirety of its existence in the archaic period, it was the largest and most important close-by Greek polis from a Caucasian perspective.
But there are also two specific linguistic reasons to believe the loan was early. First, the /dz/ reflects the Classical and not Koine pronunciation of Greek zeta, which later shifted to /z/. This gives a terminus ante quem of around the 4th century BC and not much later.
Second, in Megrelian and Laz sonorant consonants like /r l m n/ in tonic syllables are rather unstable; they tend to be deleted, but also inserted sporadically. This happens in native verb morphology but also loan words. A late ex is თამბაქო tambako from Italian tobacco.
So it seems likely that a Greek word referring to an archaic polis on the Bosporus was borrowed in the Archaic/Classical period into Megrelian or a western Georgian dialect and underwent sonorant epenthesis to produce Georgian ბერძენი berdzeni and Megrelian ბერძემი berdzemi.
This was then borrowed into preliterary Abkhaz to form Барзентәыла Barzent’wəla 'Greece' -- unless indeed the sound-change happened in Abkhaz-Adyghean, and was then loaned into Kartvelian. In either case, it happened in the West, where the Greeks lived and traded.
So that in brief is the argument for its origin. But there are problems! The most important is that the medieval Byzantines did not generally refer to their own state as Byzantium. They normally called it Βασιλεία τῶν Ῥωμαίων 'Empire of the Romans' or just Ῥωμανία 'Romania'.
There are 2 responses to this. The first is the Byzantines never forgot the older name of their city, even if for official purposes they called it Constantinopolis. The normal way city-dwellers referred to it was really neither, just Πόλις 'the City' (-bul in Istanbul).
Second, even if the Byzantines did not use Byzantion to refer to their empire, this would not prevent the Georgians from doing so. The text mentioned above says "მიქაელ... მეფობდა სამეფოსა ბერძენთასა" '[Emperor] Michael ruled the Empire of the Byzantines'.
Another issue is that traditionally Georgians have said ბერძენი berdzeni comes from ბრძენი brdzeni 'wise', presumably seeing the Greeks as the source of philosophy. This is very problematic semantically, since early Georgian sources usually praise Greek religion, not philosophy.
But there is another reason to doubt it: this is that the word ბრძენი brdzeni actually is not Kartvelian, but a loanword from Nakh-Daghestanian: cf Udi bilij- 'wise', and the probable cognate in Tsova-Tush -abc' 'know'. No Greek connotations. It is in fact just a folk-etymology.
In fact, ბრძენი brdzeni is not attested until about 1 century *later*. This directly undermines the traditional explanation. The best explanation then is one that unites what we know about Greek exonymy, Greek historical sound-change, and the context of Georgian attestation.
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