I took a short road trip to Pittsburg, NH, the largest town in New England — by area at least, I think the town has less than one thousand people but makes up over 200 miles. I drove up and down route 3 from Pittsburg to the Canadian border a few times with the moose being spotted in late evening, early morning, and night. I also had a brief view of a black bear crossing Mallogway Road. East islet Road is worth driving if you like grouse, hawks, or just want to see some streams, bogs, and lakes.. would also be a nice place to canoe or kayak. I stayed at deer mountain campground directly off route 3 perfect for moose viewing. The 4th connecticut lake is an interesting hike with views into Canada and a number of Canada Jays. Be careful driving around there, I saw many moose and deer in the area. I would recommend driving slower than you think you need to because of the moose/deer and also because of rocks on the dirt side roads.
Short moose video (listen to them walking) https://youtu.be/jFd8uuEgpfo