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To be honest, I actually enjoyed all the sound tracks present in Heartgold and Soulsilver, whether it was the up-to-date modern version, or the original using the Gameboy Sounds. Each one reminded me of when I was younger playing through Gold and Crystal versions (as well as Red and Yellow version to an extent too).
My favourite HG/SS music by far is the Kanto Gym Leader Battle theme. An intense battle. I always left my DS on just to listen to that heartracing music. Never could get over the music and never will.
route one and the classic pokemon center is pure nostalgia but I did also love Red/Lance theme. However the real winner has to be the Team Rocket music. Both during and outside battle. I would just stand in the radio tower for ages listning to that music.