Of course they do. But they are primarily for flavor (think salt and pepper, like seasonings to enhance the beer) and not pH control.
If you look at your spreadsheet there, adding 10 grams of CaSO4 will change the makeup of the ions of the water far more than the pH. If you want to reduce the pH from a very high pH to a mash pH like the OP mentioned to 5.2 or so you'd need so much gypsum that the beer would be undrinkable.
Think of cooking. A little garlic, a little oregano- great spaghetti. A pound of oregano, not so much. The base is tomato, and the seasonings will enhance that. With beer, the base is water, and the salts ("seasonings") will enhance, but it's not the primary way to control a very high mash pH.