I feel like AH is ready for something a little more complex/bigger than Vanilla MC, with the individual mod LPs showing that. Personally, I've enjoyed all of the modded ones and I think that they could start a recurring Modded series.
They could recreate Achievement City in a PC world (Let's be real, it would be easy to recreate it in creative), and branch Let's Plays into accomplishing certain tasks (New dimension, certain block).
Now for the Mod List:
General Mods:
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NEI - Recipes, Save Inventories
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WAILA - To know what they're looking at.
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Tinker's Construct (+ExtraTiC) - Allows custom made tools and weapons, and the addon allows for more materials to be used.
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Fossils a

