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I would avoid the first and second weeks of June if possible as that is gnat season. Otherwise, sunrise at the Badlands, be to the south just before dawn if it will be sunny. Lots of prairie dogs and the flowers should be blooming. The waterfalls should be running nicely that time of year south of Spearfish. Custer State Park is probably the best single area, but stay well away from the buffalo. They will certainly kill you if you get too close. They are very, very fast. Needles parkway is worth the drive.
Kent in SD