Not sure if your phone/android version is the same since that info was not provided.
On my Galaxy S 4 running 4.2.2 (your phone may vary from this some but in general should be similar):
Open phone dialer (keypad)
Press menu button (to the left of the home button)
Select Speed dial setting
Select the key I was to add speed dial to
Search contacts for contact to add and select
Additional note: long pressing a button with an existing contract will bring up a menu to replace or remove that contract from that key.
If you have any more questions about this you will need to create a new question, you are welcome to link to this one or register with the forum so you can reply here.
Also, if any other contributors know of another phone having a very different path to edit speed dail settings, additional replies would be appropriate.
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