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Heart Gold/Gold, because of the amount of content, particularly in terms of breeding, the day/night cycle, the geography of the region and the story, and still had the feeling of "What's around the corner? What comes next?" that really made Pokemon a great experience, which I felt lacked in the Sapphire/Diamond generations. I felt being able to play through Kanto after Johto was great, too. I will say I have been massively impressed by Black, and if I ever find the time to go through the post-story content, it may come in at a very close second.