ASP.NET 3.5 and above only

Obout.Ajax.UI Controls - HTML Editor - How to make Custom top toolbar in VS

Open Properties for Editor control, expand TopToolbar and set Appearance to custom:



Call CommonButton Collection Editor:



Add the buttons you want to the collection:

 

After your buttons collection is filled, press OK button and the Editor control will be rerendered.
Now, if you call CommonButton Collection Editor again, you will see the following:

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