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Strange, since my recollection is that the original D&D got a lot of their alignment stuff from Elric of Melniboné and other similar book series. The first book of that series was published in 1972. Now those books were about Law vs Chaos, but still it seems that their claim would be weak.
Yep, I believe the first big one for that (Law vs. Chaos) was Three Hearts and Three Lions (1961) by Poul Anderson.