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I've always loved Starálfur, and Svefn-g-englar. Flugufrelsarinn is nice as well. Ágætis byrjun is by far their best album, I think. Although I haven't really listened much to Valtari yet.
Sadly, Agaetis byrjun is the only album of theirs I don't own (and that includes the Inni live album, Hvarf/Heim, and every other more obscure release except the Saeglopur Japan Tour EP), so I haven't included any of its songs because I'm afraid of mp3-based services like Grooveshark. I listened to the album once through a friend and most of its songs are on Inni or in Heima at some point, but I don't want to make conclusions until I've heard the studio versions.
Up until recently I liked () the best of all the albums, but I'm coming around to
Med sud i eyrum vid spilium endulaust despite the poppier sound of about half its tracks. Valtari is interesting and is definitely Sigur Ros, but it's noticeably lacking in bowed guitar. I doubt they'll be doing much from Valtari live (actually, the band has said as much), because it simply involves less real instrumentation and more ambient effects.
In another note, I'm a bit afraid of what will be in the next album slated for release this year, since Kjartan left the band (he joined after Von and before Agaetis byrjun, and was almost singlehandedly responsible for the transformation in the band's sound rounding out the end of the millenium).
Also, kudos to you for spelling (or at least copy-pasting) the names of everything correctly with accents and everything, something I was too lazy to consider.