Ugh, this is a hard one! I'd say either HG/SS or B2/W2. Definitely both amazing games. But I think I'm going to have to go with HG/SS. I really loved these games. They had so many stuff added from other games, and even going as far as pretty much implementing Crystal into both. I'm also going to mention the obvious; walking Pokémon! Really though, walking Pokémon was an amazing addition. It gave a different level of emotion to your Pokémon, and I'm sure it must've been hard for Gamefreak to implement so many sprites, plus the shiny editions! There's also the Bug-Catching Contest. Definitely an original idea I haven't really seen in any other regions besides Johto. The concept of capturing a Pokémon for a contest and winning depending on what Pokémon you caught + level would've been worn out if it was done in other games, but it wasn't! That is purely what makes it original.
I'm pretty sure the Pokéathlon was great too! I enjoyed this far too much. It's slightly similar to the Bug-Catching Contest, but also very different! I like how they implemented an olympics for Pokémon, it was definitely time! The fact that there was quite a few minigames made it better. I don't exactly remember, but I believe you could even challenge some Gym Leaders in the tournaments! I really liked this. It made it all the more intimadating to enter the olympics, and when you outwon the person by just a speck, it definitely made you feel accomplished. I'd call it the counterpart of Contests.
I could keep going on about this. I do know that they implemented the Battle Frontier from Platinum into HG/SS, but I wasn't to keen on the battle streak stuff as I could NEVER reach a Frontier Brain. Never got to hear that awesome music in-game. :( But nevertheless, it was an amazing addition as it was purely an add-on, and most people seemed to be delighted with it!
And there's 2 regions! I am going to admit Kanto was slightly confusing and bland, but when you just find out you can explore a whole new bunch of cities and routes after thinking you've completed the game, you get a rush of hype and excitedly, enter Kanto! I remember doing that the first time, but I did know about the Kanto post-game lol.
But that's pretty much it! I don't want to keep blabbering on, I think I've wrote enough. :)