"While he was never King of England himself, Alfred paved the way..."
To claim Alfred wasn't the first King of England reveal a gross ignorance of history. No, he wasn't king of the modern day extent of England, but nor were many accepted kings of mediaeval France. Indeed Alfred controlled as much a proportion of modern day England as many of them did of what is now modern France - and the same could be said for many other countries king-lists. Alfred is the first to be accepted during his reign as king of all the free Anglo-Saxon territories, rather than just the biggest of a bunch of squabbling tribal kings & kingdoms. As such he is the founder of England as a nation state.
But it goes much, MUCH further than that. He had not only saved the last Anglo-Saxon territory from being swallowed by the Danes, he made English the official language (translating many books himself), he created the first national education system through his grammar schools, and oversaw their curricula. And much of the World (and certainly the English-speaking countries) owe him for creating The Common Law - the first codified legal system to apply to every one in the country great or small (even slaves had rights and could earn money and have ownerhip of things, making them more a protected serf rather than a slave). And many of his basic legal concepts and rights exist to this day and have spread across the free World. As such, he seen as both saviour and spiritual founder of England's national identity, laws & language, and hence not just the first king of England, but the only one to be titled "the Great".