This can sometimes be a good idea. But it isn't without downsides. Now your config file is Python and capable of doing anything Python can do (which isn't necessarily a good idea), it's no longer safe, you now have to deal with shitty Python tooling, you might have to debug crashes/lockups in your config files, you can no long switch implementation languages, etc. etc.

It isn't a magic solution.

Not that this is a magic or even a good solution, I just wanted to mention that sometimes you already have the thing you are looking for directly under your nose.

I never had any project were a toml config wasn't enough.