Please keep in mind that this is in the context of taking the CPU card components completely out of the equation. Imagine the card can cope with it.
All chips can go a little over spec, but how much can pretty much all masks of 68060s handle with basic fan/heatsink cooling?
Is 66MHz pretty much guaranteed? (only 16MHz, I actually have an old XC marked 66MHz)
How far can you get at 3.3v?
Does 80MHz+ really require upping the voltage?
Thanks
My Apollo was the 66MHz (factory overclocked) revision 5 XC68060RC50. At least I think it was revision 5. I wanted more speed so I tried 75MHz and it booted, but it would crash before completing the boot process. I could even boot with no startup-sequence and go into workbench that way but it wasn't long before it crashed. I then tried upping the voltage a little (thanks to Cosmos for the mod), but it made no difference in my case, so I un-did the mod. So I decided to buy a revision 6 latest mask 060, and clocked it at 80MHz. It worked first time and I've never looked back since.
I did measure the voltage on the (unmodified) regulator but I can't remember exactly what it was. I have a feeling it was higher than 3.3v...maybe 3.62v, so I'm not sure whether 3.3v would work at 80MHz. Then again, how accurate is my meter? It was only cheap and I've had it 14 years.
But looking at it from another perspective, my Apollo was factory overclocked so they could have cherry picked a beefier regulator pcb to begin with.
My advise, try overclocking without doing the voltage mod. If 66MHz isn't working for you, then you might want to try the mod. But grab the latest mask 060 if you can, as 80MHz makes a nice Amiga.