Part of the premise of your question is wrong—the idea of zombies as the "walking dead" is an old one, and had also featured in earlier films. For example, on google books I found that the book Cuba and Porto Rico, which according to the title page is from 1898, says on page 395:
Another strong feature of obis is the belief in haunts. The negroes believe that not only the spirit but the person of the dead, in modified form, returns to trouble the living. These more nearly correspond to the shades of the ancient Greeks, having body and substance, than to our conception of spirits which are without them. These shades are known in Jamaica as "duppies," in Martinique as "zombi," in Antigua and Barbados as "jumbies," and in America as "harnts." ... Dead children are especially liable to return as duppies to haunt the mother, who, even though she may have been the tenderest of creatures, always recalls some act of omission or commission on her part which will cause the child to return and punish her. To prevent this, they are very particular to put heavy weights on the graves; otherwise they will awake some night to find the duppy sitting upon the foot of their bed.
On the other hand, the book Two years in the French West Indies from 1890 (which seems to be nonfiction from the preface) recounts on page 188 (from the chapter 'Martinique sketches', matching the claim above that the term 'zombi' is from that island) an interview with a local girl named Adou who says "I do not want to go by that cemetary because of the dead folk;—the dead folk will bar the way, and I cannot get back again", and when the writer asks "But are the dead folk zombis, Adou?" she says "No; the moun-mò are not zombis. The zombis go everywhere: the dead folk remain in the graveyard." So either beliefs about the nature of zombis differed, or one of these reports on the beliefs is inaccurate. Still, the first quote does at least show that some outsiders understood the zombi stories in Martinique to refer to the dead that have physically returned to "trouble the living".
As for film, the first feature-length zombie film, which probably popularized the legend of the zombie for mass audiences, was White Zombie from 1932 (starring Béla Lugosi, famous for his portrayal of Dracula), and it featured a voodoo master named "Murder Legendre" turning a living woman into a zombie, but only after she had apparently died--from the wikipedia plot description:
Beaumont agrees and surreptitiously gives the potion to Madeleine. Shortly after Madeleine and Neil's wedding ceremony, the potion takes effect on Madeleine and she appears to die. After her funeral, Murder and Charles enter Madeleine's tomb at night and Murder revives her as a zombie.
If you go to wikipedia's List of zombie films and click the "Year" text in the chart to order the films by release date, there are some early films where the zombies are definitely reanimated corpses, for example the film Revenge of the Zombies (1943) has an extended plot description on this page which says "In an overgrown cemetery somewhere in the Louisiana bayou, a curiously stiff black man with huge, white, pencil-eraser-like hair (Comes Midnight’s James Basket) uses an odd, hooting call to summon a pack of corpses from their graves." This movie was a sequel to King of the Zombies (1941), which is on youtube here, you can see at 14:24 that one character says "wait'll you see the zombies", and when asked what they are, she says "dead folks what walks around" (and the zombies appear very shortly after that). Also note that Night of the Living Dead was not the first to suggest some alien influence rather than voodoo was responsible for reanimating the dead, as this idea had been featured in Plan 9 From Outer Space (1959) and The Earth Dies Screaming (1964), though I don't think either film referred to the dead as "zombies" (but neither did Night of the Living Dead).
As for Romero, this article has some details on how he and his co-writer on Night of the Living Dead, John Russo, came up with their particular version of the zombie:
As John Russo, who co-wrote NOTLD with Romero, wrote in his book Scare Tactics, “What we did was give the old zombie legend a new twist. We made our zombies into cannibals–eaters of human flesh. And in our movie there were lots of them. They were weak and slow – moving as individuals, but they had strength of numbers on their side. Conceptually what we had done was cross the zombie myth with aspects of the vampire and werewolf myths to come up with something new.”
Not that this was intentional, mind you. When Romero and Russo got together to come up with an idea for a horror movie, they were working on separate typewriters in different rooms. A cemetery seemed a good place to start a horror story, and Romero came up with an opening with people getting attacked in a graveyard, but it wasn’t clear who was attacking them. Russo suggested they could be dead people, and then they went back to an earlier idea of aliens coming to earth looking for human flesh to eat, which is where the cannibal element came from.