If we were including the PC-98 games, then I would probably say the original version of the Touhou 1 soundtrack, since it's kind of primitive compared to everything after (including its much better version in Touhou 5 and Akyu's Untouched Score).
But since we're not including the PC-98 games, I think Hidden Star in Four Seasons has the worst soundtrack, since the style that most of it uses doesn't really work in my opinion (the title screen music was pretty good, why couldn't ZUN have just made the rest of the soundtrack using a style closer to what he used there?), alongside my opinion that some music tracks don't fit with the stage/boss they're used for (such as the music for the second stage).
A three way tie between 16, 17 and 18. There are about 3-5 tracks max I actually remember fondly from playing them, partly due to zuns change in style.
If I had to rank the three from favorite to least favorite, it would be 17-16-18. A shame because immemorial marketeers is one of my favorite tracks from the series.
For me, 16 has a lot of tracks that aren't particularly memorable. I really don't like piling onto the newer games much, because there are quite a few tracks I like overall.
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