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If you decorate with skulls or have built a wither structure, an axe makes taking the skulls down quicker.

Pick an axe, ideally with Efficiency, and put it in your hotbar.
Make sure the area is safe. If you are removing skulls from an old wither build, be sure no wither is active.

1. Stand where you can reach the skulls without leaning over edges.

2. Select the axe.

3. Break each skull one by one. Wall-mounted and floor-standing skulls both respond to the axe.

4. Collect the dropped items. Walk over them, or move closer if your inventory is full.

5. Store the skulls in a chest or reuse them elsewhere.

Skulls drop as items when broken, so you can reposition a display instead of rebuilding it from scratch.
The axe only speeds up the breaking. It does not alter the drop or add any new behavior.
For anything that is not a skull, such as the blocks the skulls sit on, switch to the tool that suits that block.