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The Hot Fives and Hot Sevens is the body of work that most jazz critics would say to be his greatest.
Given the age of those recordings, the sound quality won't be great, but don't let that keep you away.
After that, there are a lot of albums that he made, over a period of decades, that are very good. "Louis Armstrong Plays W.C. Handy" is one that comes to mind.
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