My experience was pretty hit or miss, and mostly I ended up with an mismash of semi-random keybindings which is sort of the opposite of what I was shooting for. On the Mac developers have done a remarkably good job of adhering to a consistent set of shortcuts (down to things like Command-, for preferences).
The other issue is that most apps don't make it straightforward to bulk re-assign keybindings from Control to Super, and last I checked it was impossible to turn off menu accelerators for Gtk+ based apps (e.g., Alt+F to bring up the file menu in Firefox).
Most of the time what I want is to map Command->Super and Option->Meta, and have Super replace Control in all GUI app keyboard shortcuts leaving Control available for command-line apps, in general.