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Have you rebooted the Mac this problem is on lately? I did have a bit of trouble the other day where I could see the Mac from my iPod in the send settings step, but couldn't get any further. The issue turned out to be that I had run out of disk space and the process that runs the Bonjour sync server couldn't do anything useful except advertise its presence (it couldn't actually share the settings). Quitting the apps which had gobbled up too much swap space and restarting made everything happy again. Might be worth a shot just to rule out the possibility that something has happened to the sync server process, though I doubt it is the reason. Just to clarify: on your iPhone, after you've pushed the Share Settings button on your desktop, you never see "Bill Palmer@Bill-Palmer's-Macbook" (well, obviously the username and machine name will be different), you just see "Searching...", right?

Brian is suggesting a computer-to-computer wireless network, not cabling the iPhone up with the USB sync/charging cable, which doesn't do anything relevant here. Does the Mac in question have a wifi card installed?