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I know that title seems too cutesy and I apologize for that. It is both a historical oddity and a signifier of our general Orientalist indifference toward the peoples of the Middle East that the nation (kingdom, empire, whatever it was at any particular point in history) of Iran was never officially called "Iran" by anybody other than Iranians until 1935. Iranians, on the other hand, had been calling it "Iran" for millennia.
It fell to Reza Shah Pahlavi (d. 1944) to point out to the rest of the world that they were getting Iran's name wrong, which he did in December 1934. He made a public request/demand that, as of the next Iranian New Year (Nowruz), all foreign governments should henceforth stop referring to his country by the name "Persia" and start calling it "Iran." Often you'll see Western writers describe this as something like "Reza Shah changed the name of the country from Persia to Iran," but that's simply wrong. "Persia" was, for the most part, what's known as an "exonym," which is the term used when a group, place, language, or some other national feature is given a different name by people who aren't part of that group, or don't live in that place, or don't speak that language, or all of the above.
Reza Shah, circa 1940 (Wikimedia Commons)
With all due respect to Herodotus or whichever Greek writer convinced the rest of the world that the land between Mesopotamia and the Indus River was properly called "Persia," this was usually not how the people who lived there described it. You can go back to inscriptions from the second century CE that refer to the place as "Iran," and that word or its variants (Iranshahr, Iran-zamin) go back far earlier than that. The ethnic identifier "Aryan," from which "Iran" derives, can be found in use as far back as the Achaemenid period (500s BCE) and in the Zoroastrian scripture, the Avesta, which reflects a tradition that goes back earlier than that (though the earliest extant complete copy of the Avesta dates to the 14th century). The label "Persia" is essentially a historical error. Cyrus the Great (d. 530 BCE), who founded the Achaemenid dynasty, started out as the king of Parsa, the region of southern Iran that is today called Fars, the "p" having been swapped out for an "f" when the Arabs conquered it because Arabic has no "p" sound. Greek writers, demonstrating that a little knowledge really can be a dangerous thing, applied the word Parsa to the entirety of Cyrus's domains, even though the actual Parsa only referred to that one part of his vast empire.
After the Arab conquests, the whole idea of referring to historical Iran by a single name became defunct, as the former "Persian" Empire was broken up into several provinces: Fars, for example; Iraq al-Ajam ("foreign Iraq"), the region in central-western Iran next door to Mesopotamia (if you're wondering, Mesopotamia was called "Arab Iraq," Iraq al-Arab); Sistan, in southeastern Iran; Khurasan, in northeastern Iran (including most of modern Afghanistan); Mazandaran, on the southern Caspian shore; and so on. Once the caliphate fell in 1258 and really independent kingdoms arose once again in Iran, the concept of "Iran" as a complete geographical unit became relevant once more. The rise of the Safavid dynasty in 1501 really marks the return of "Iran" to the world in the form we know it today, although the Safavids, during their heyday, ruled a territory that was considerably larger than the modern nation of Iran.
Why did Reza Shah ask the international community to start calling Iran by its proper name? Yes it was more accurate, but he also had geopolitical reasons for doing so, and unfortunately they involve the Nazis.
It would be wrong to describe Reza Shah as "pro-Nazi," because of course that carries all kinds of connotations in terms of ideology and racial identity. You need evidence to support a charge like that and in Reza Shah's case it's lacking. The Jewish community in Iran, though not large, was not ill-treated under the Pahlavis, so on that point alone I think we can say Reza Shah was not pro-Nazi. He was, however, pro-German. Or at least he was, by the mid-1930s, growing increasingly anti-British, and for a Middle Eastern head of state looking for a European patron in the 1930s, being "anti-British" meant that you pretty much had to be "pro-German." So he and the Nazis had at least one thing in common. As "Aryan" fever gripped Germany, the Nazis convinced the shah to emphasize the name "Iran," which as I noted above derives from the same Old Iranian word whence we get "Aryan." This was supposed to affirm some sort of historical bond between the Germans and the Iranians, and lend historical depth to the Nazis' idea of a pure "Aryan" race. In return for lending some legitimacy to Nazi race science, Reza got closer ties with the enemy of his enemy.
Reza may also have wanted to emphasize Iran's roots as a display of domestic legitimacy, highlighting the fact that he was really the first "Iranian" ruler of "Iran" since the Arab conquests all the way back in the seventh century. The Safavids, who get credit for restoring "Iran" as a unique and whole political entity after it had disappeared with the fall of the Sasanian Dynasty, were of mixed ancestry but primarily Kurdish. Kurds are an Iranic people but they're not Iranian per se, and anyway the Safavids' authority rested heavily on the strength of their devoted Qizilbash cavalry, which was primarily Turkic. When the Safavids fell, it was those Turkic Qizilbash tribes that took over—first the Afsharid Dynasty of Nader Shah and then the Qajar dynasty, which ruled Iran from the late 18th century until Reza Shah's ascent to the throne. Maybe Reza was trying to aggrandize himself by assuming the mantle of a truly "Iranian" ruler.
If you look hard enough, even today you can find arguments about whether the country should properly be called "Persia" or "Iran." My sense is that Iranian (or Persian, I guess) folks who prefer "Persia" do so as a way to hearken back to the ancient empire as opposed to the image of the modern Islamic Republic. This phenomenon also gives rise to some of the silliest of the generally silly mainstream American media takes on Iran, like this thing from The Daily Beast called "Are We Negotiating with Iran or Persia?" One of those is supposed to be bad, I guess, but I haven't actually read the piece and I am completely unable to make myself care what the point is, assuming there is one. For me I'm on the "Iran" side of this argument, and I think generally speaking that's where the historical record lies as well.