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My favorite artists so far are:

Other chiptune/8-bit/etc artists I have in my library are:
Twilight Electric
I Fight Dragons
Henry Homesweet
Bit Shifter
Megaman 1 through 6 OST
Organic Computer

I'd love to have some recommendations. I'd prefer for them to sound similar to my favorite artists, but I'll give anything a try. Some of the artists I've listed here aren't exactly chiptune, anyway. :P

My favorite song so far:
Post edited February 10, 2012 by Chevve
Ratatat is all I can add. Their s/t and LP3 are great. That youtube link you gave was really good too.

You might also like Son of Robot - Spring09 EP.
Take a look at 8-Bit Collective. I've got a 'best of' collection from them; it's dated from 6/06 to 6/11 and has just over 4,000 tunes.

I'm moderator on a site that hosts legal torrents, and you can get it from there. Here's a link to it.
4mat has some good stuff.
You can nab all of his stuff on free music archive.
Or you could hit up his bandcamp if you want FLAC.
I know his bandcamp page doesn't have all of his music, though, but it does have all of his main albums for free.
Perhaps you would enjoy some Impostor Nostalgia. The album isn't free, but you can listen to all the tracks as samples. Not all the tracks are pure chiptune, though (if any, they might be impostors and I really couldn't tell).

There's also FantomenK.

I am required by love (and justice) to encourage you to give this a try, even if it's "Piano + NES".
For "pure chiptune" I would really recommend PPPPPP, I personally also listen a lot to Impeccable Micro now. :)
The Mega Man 9 OST is awesome, especially Flash in the Dark (Wily 1.)
I actually watched these guys live yesterday. They might tickle your fancy as well (that is the band 047)

you can download some of this tracks for free there
saldite already suggested 4mat so I'll suggest Dubmood
Dubmood - Sleepless (Cydonian Sky 2)
Dubmood - Afterburner
Dubmood - Mario Airlines

Also one of my favorite songs by Quazar
Quazar - Funky Stars (aka Hybrid song 2:20)
and Dubmood's cover of it
Dubmood - Hybrid Funky Stars

Modland ftp for lots of Fasttracker 2 modules
Post edited February 11, 2012 by Sude
I assume You've already found 8bitpeoples, given the artists in your library, but I include the link just in case you found them elsewhere.
Post edited February 11, 2012 by Miaghstir
Pterodactyl Squad/ if you don't already know about them.

Also, Rygar soundtrack. I can't remember shit from games I played 5 years ago but I can recognize chip music I haven't heard in over ten years from games I played as a kid in .1 seconds. For some reason, I like it as workout music.
Zan-zan-zawa-veia, Souleye (VVVVVV), Brother Android, b4kn and Phlogiston
Check out the new Indie Game Music Bundle, maybe you'll find some chiptunes among these soundtracks. There's also one of Disasterpeace, but you probably know that already?