Yes, use that mode if you want the best image quality at 60fps. It's the mode that uses PSSR.
Quality mode (which is also on base PS5) might have some graphical advantages in some areas (like foliage pop-in distance and a bit better image stability), but the graphical differences between the two modes are minimal and Versatility mode is actually sharper than Quality mode and it runs at 60fps. Quality mode only runs at 30fps. The other performance modes are garbage so don't bother with them.