I'm going to be staying on Victoria Island in late September, and what are some good places to drive to during my three day stay?
My guess is you're referring to Vancouver Island (where Victoria BC, but not Vancouver BC, is located), rather than the Victoria Island in the Arctic, or one in some other province. Right?
In addition to the short hop down to the Mile 0 (still not metric) of the Trans-Canada Highway on the south side of Victoria, there's also Tofino on the west coast of Vancouver Island for a more distant day trip to a small coastal town with a scenic highway leading to it. I've also been to the less interesting Port Hardy at the north tip of the island, and Comox and Nanaimo on the east coast, just for the ferries to or from the BC mainland.
A small rest/scenic area on the northbound TCH between Victoria and Nanaimo has a cool totem pole. No direct access to the rest area from the southbound TCH.
I can't help on your other question about ferries between Port Angeles and Victoria, since my travels to and from Victoria were on the BC Ferries system, or once on the Washington State Ferries route through the San Juan Islands.
I only went to Victoria and back to Nanaimo, and obviously you'll have the sights of Victoria covered. Hit up the west shore, definitely, and on a different day, head all the way north. Both west and north sides are what I've heard to be the best of the island, both online and from residents.
I recommend the Pacific Marine Circle Route, 158 miles. One segment wasn't fully paved until just a few years ago, so it's relatively new on the tourism circuit. Easily done in a long afternoon, although much of the coastal road is fairly slow going. Essentially no services for the middle 140km.
http://www.hellobc.com/driving-routes/19/pacific-marine-circle-route.aspx
Hmmm.... that route looks like something that I would do on a full tank of gas.
I have never been out that way personally, but I have heard a lot of people rave about Tofino, on the western coast. It's a fair distance from Victoria though.