Part of the problem is just that this is a brand new rather large set of changes that just have some bugs right now more than that it's you doing something wrong ... It's just going to take a couple builds to get the kinks worked out.

So Q&A:
Here's the tag that ended up on the playlist (saves having upload a jpg):
tagletter,title:artist~tag,title:artist~tag,source:source~search,tracknr:(type = "tune")

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So the result is that some of the albums sort just fine, some of them do the alphabetical/numerical sort (1, 10, 11, 2...) and a few sorted in a bizarre way?

The numerical sort problem is fixed for 64 .. When

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Did I do it right? Should I do Albums sorted by Title (based on your comment that Title changes context), or Album sorted by album?

For tag soup layers, title should always equal the tag you're souping on. So if you have an artist tag layer, then the title should be the same as the artist tag. Same for album, year, etc. So you should be able to interchangeably use album or title. Now the interesting point here is that there is definitely a different implementation for those two paths -- title uses a more optimized path, so it's possible the non-optimized path has a bug in it. I'll try to set this up and see if I get the same problem. 64 is getting a bit of an overhaul in this department actually to support reordering of playlists when rolling up tags to the playlists, so I'll just make sure to test this. If you have a chance, it actually is kind of helpful to see the screenshot -- what seems random may actually be meaningful when I see the exact order in case I can't reproduce the exact problem on mine -- I can try to setup the same values that you have in your sort.

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Also, should the last one be "all sorted by track #", or "tracks sort list" sorted by track #?

Technically you should get the same behavior ... All is defined as "type = tune", but tag layers only allow type = tune anyway by definition, so All just does extra work that you don't really need to do (it does that one last restriction that is always true). Tracks Sort layer is just a slightly more optimal layer to use for the bottom layer.