^Well, the question is whether Spock was the first, so anything that doesn't predate 1966 wouldn't address the question. (I'm not counting the pilots because those wouldn't qualify as "regular TV appearances.")
Although I think we've fully established by now that the answer is a definitive "no."
Just to muse over the question, though, I'm not sure I'd count ghosts as nonhumans, because they were formerly human and still have human personas. Essentially it's a human consciousness without a human body, so I'd call that something semihuman rather than nonhuman. As for angels, that depends. Is it the pop mythology where angels are former human beings who died and earned wings in the afterlife, or the more Biblical definition of a subordinate level of supernatural beings? I would imagine most angel-related TV shows would favor the former, but I haven't seen most of them so I couldn't be sure.