Pull up any existing vegetation. Although mulch will eventually kill grass or plants underneath it, some can survive and will poke through, ruining the effect. Pull up or clip down the grass in the area where you want your border.
Lay landscaping fabric down over the area for your border. This will also help prevent weeds or grass from poking up through your mulch. Black landscaping fabric is best for this application. Cut the fabric to the size of your border and lay it down. Use heavy stones to secure the edges until you are done.
Pour the mulch out over the landscaping fabric. It is OK to overlap some of the surrounding area with mulch since this is a natural border and not a straight or set border. Pour the mulch out evenly, and go through it with your hands to separate any large clumps.
Rake over the mulch if necessary to even it out. Although this is a natural border, you still want some uniformity so the finished result looks polished. Smooth out any rough spots, add more mulch in low areas and try to get it as even as possible. Remove your stones and fill in the areas that were underneath them with mulch.
Wet down the mulch. Natural mulch should be somewhat moist when you take it out of the bag, but it will dry out quickly. Wet it down with water to help keep it in the right position. You may have to wet the mulch down occasionally, particularly if you live in a windy area.