I mean everything about Auntie Ethel and Raphael - those interactions are just so entertaining. They should be the main villains in the game
Playing instruments and gatehr crowds as a bard
Speak with Animals - 'nuff said. They are the stars of the game
The music - I cried at the Nightsong scene, that didn't ever happen to me in a video game
Arabellas interactions with Withers - just the best
Barcus and his dialogues - he truely feels like a friend made on the road
And I gagree with rodeafant: the three Thorms are jsut creepy in a very good way, really had me on edge the first playthrough.
The hommage to H.P. Lovecraft with the Necromancy aka Necronomicon
