We actually took the ferry from Portland, Maine to Yarmouth and circumnavigated the entire province in 11 days, staying at B&B's the whole time. You're right, it is all beautiful.
Highlights were the Cabot Trail, of course; visiting a whisky distillery; Louisbourg; going down in a coal mine that stretched out under the Atlantic; a birdwatching boat trip out to some small unihabited islets; catching a glimpse of the Newfoundland mountains from a tiny fishing village on the rockbound northeastern tip of Cape Breton; a sailing excursion in Halifax on that schooner that is on the dime (the Bluenose, I think); and rafting the Shubenacadie River at the tip of the Bay of Fundy, riding the incoming tide 12 miles upriver.