I was struggling to find the typeface used for this album art, and was about to assume it to be one-off lettering when I stumbled on Coro Moonin Photo-Lettering’s One Line Manual of Styles (1971). Typeface names prefixed with the designer’s last name were common in the PLINC library, though in this case it could be that the font was not by Columbia Records designer Ron Coro, but made for him. The name also indicates that it was developed specifically for this project. These are only guesses, but PLINC frequently supplied the type for Columbia in the 1960s–70s, including many sleeves by Coro and John Berg.
Type aside, Moondog (born Louis Thomas Hardin) is a fascinating story in his own right, and I advise getting to know him and his work. A documentary film about his life is currently in production.