So in order for me to make Daedric Armor Items, as I have 90 smithing now, I need to acquire Daedric Hearts, however Arcadia never seems to have any in stock, any suggestions?

That shady guy at the mage college has one.

I understand that doing the Dawnstar Museum quest you can get up to four Daedra Hearts, anyone know of any other ways?

I saw one for sell, I believe it was on Whiterun in the store that sells all kind of junk but I'm not sure if it was there.

Kill Dremora.