Bang on with Comus and Spirogyra (although I might work my way up/down to Comus) . Try also the "Early Morning Hush" compilation on Castle Records which features a lot of rare and wonderful late 60s/early 70s stuff and the "Strange Folk" comp which is a mixtureof old and newish.
Also try
The Incredible String Band - Hangman's Beautiful Daughter
- 5000 spirits
Forest - Full Circle
Newer stuff?
Espers - any of the three albums. If I had to pick one I'd go for the mini-album of cover versions called (I think Weed Tree) but they're all good.
Tuung - yep, I've spelt it right!
Selectively download Devandra Banhart and the Wyrd folk crew, some of which is hit and miss it hasto be said
Oh and pretty much anything else from Stevo's list
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