iTunes Home Sharing would only be a possiblity if both computers used the same online iTunes account.*
iTunes 'regular' sharing (iTunes > Preferences > Sharing tab) would allow each computer to see and play the other's library (if the other computer was running and iTunes was open), but the portable iDevices could still only sync to and store the contents of one computer's library at any one time.
If the two libraries were consolidated to one computer, then each iDevice would have to sync to the main library computer (as you can't sync a shared library from another computer), and all future iTunes online purchases, other downloaded files, CD rips and library maintenance would have to performed on that computer. The other computer's only function would be iTunes playback of the shared library on the main library computer.
*Under the one-computer-consolidated-library scenario there wouldn't be much point in having a separate iTunes account on the other computer, because all library additions would need to be performed on the main computer anyway. So if both computers used the same iTunes account, Home Sharing could be used, but the only advantage in your scenario would be that the iDevices could stream the main computer's library via WiFi to the iDevice because (a) the library is too large to fit on the iDevice or (b) you wanted to playback the main library on the iDevice without syncing, and of course would only be a feature for local WiFi use.
I'm not a Cloud user, so there may be a scenario usable with the iCloud, but I think you would still be limited to a single iTunes account.
Steve