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After a few years... I think it's "The Signs". It is just the best song ever written. But I love most of the GG songs.
I also loved 9669 by The Joy Formidable that played in Double Identity when Serena was telling Blair that she'll regret it if she doesn't talk to Chuck.
Stripper by Soho Dolls (when Chuck decides to buy the Club Victrola) and URA Fever by the Kills (when Serena says "I killed someone" to Blair). They are both from Season One.
Oh and I forgot:
Come Home - One Republic
With Me - Sum 41
They are also from Season One.
I think "I can feel a hot one" is probably the best song that's been featured on GG - I'm a sucker for a beautiful, yet mournful tune.
The Only Exception-Paramore
I definitely thought that the Season 1 songs were the best. They were all very interesting different. Season 2 was OK. Season 3...hmmm nothing that really caught my eye.
"I'm In Here" by Sia
(the unforgettable train station scene)
I think the best song featured in gossip girl till date is Apologize by one republic.And i also loved right round by Flo-rida.It was so perfect for the scene and it was kind of naughty too.lol.
this will be one of those songs: http://www.youtube.com/watch?v=4_yskRDrmqI
The National is just amazing!