DS icons: http://gbatemp.net/index.php?showtopic=45360 if you want to do it manually.
There was an editor called RomeR not so long ago by Kyuzumaki for all DS code and Rominator does it (RomeR was more or less integrated into Rominator) for commercial roms as I recall.
PC icons
If you mean DS roms them the cycloDS team made an app/plugin to make DS roms have their own icon in windows.
If you mean in general there are many ways but the simplest is to make a BMP file with the extension .ico and set it manually
This is one of the few times you will ever see me link to wikipedia but for once it has it correct enough: http://en.wikipedia.org/wiki/ICO_(icon_image_file_format)
To set it in an explorer window hit tools -> folder options -> file types browse to the extension you want to change and hit advanced -> choose icon and browse to the .ico file.
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