Sorry to revive an old one, but I have a similar problem.
My library has got to 181gb, and so my 2011 500gb macbookpro is struggling now.
I bought some external hard drives (WD My Book for Mac) and intended to use one for the iPhoto library, and another to back that up to. I already have a third which does the regular back up for the laptop.
Anyway, upon attempting a transfer, I had exactly the same message as Sam back in 2011, and have followed TD's advice above, except I didn't know which of the 6 options to use.
So I ticked the first, and left it to work away.
That completed, I ticked the next three options and left it - came back and "iPhoto had quit unexpectedly" - I guess I asked too much of it to do them all together.
So I've gone through options 2,3, and 4 individually. 4 (upgrading thumbnails) took around 9 hours.
I deleted the 53gb library that had moved to the EHD and emptied the trash on it, and tried another transfer.
But I still got the error code 36 message.
On the EHD, 181gb was showing in the finder window, and the EHD worked away when the library was opened, but no thumbnails or pictures were viewable, and after a refresh of the finder window, only 54 gb was actually there.
So, any suggestions?
Should I try to split the library into smaller chunks? (if I can?)
I will try option 5 in the rebuild menu, then option 6. Will update if this has any effect.
Regards, YDG.