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Do you need simultaneous access from both devices? If not then an external HDD/SSD might do it (with a regular backup routine)
If you've got that much mail and you want it synced then you should really use a suitable IMAP or Exchange server and let the local copies take care of themselves. Trying to sync large PST files will just cause you aggro, not least because unless things have changed, the sync systems don't see the deltas, so need to do the whole file each time.
Your other option is to set a delay on message deletion from the server (I'm assuming POP) so that each machine downloads their own copy. Then you just have to worry about Sent items (cc yourself) and getting the overlap right. Although if you file mail into subfolders that aspect won't replicate.
So go with option one and use a mail server technology that's designed for central access.
I had assumed Outlook would just worh with a local cached view of the onedrive storage
In the past I've tolerated my Mac laptop just seeing what currently hosted on my ISP and gmail accounts, and leaving the historical and curated folders only on my home drive, but that does catch me out sometimes when I'm away and can't find an email that has been moved to say the "Finances" pst folder, or the inevitable "Guitars" pst.
I've had work email accounts set up this kind of way in the past, but not sure what sync techniques were in play
I've always had the message deletion delay on.
So, I was basically wanting to sync a 40GB folder, with around 20 pst files in it.
I though onedrive caches locally, and it would be OK when simply avoiding using both PCs simultaneously for outlook and office generally?
Really, truly, the correct solution to what you're wanting to achieve is not to use POP to collect your mail. Then it becomes a non-issue.
Maybe I should switch to using IMAP for my main ISP-hosted email
I get that lots of people insist on using tools in ways they're explicitly not supposed to be used, but you're basically adding complexity and risk that's easy to avoid.
Obviously your choice entirely, so I'll stop banging on about it, though
If you'd been using a hammer sub-optimally for 25 years and then found out a better way, you'd change (I assume). It's just another tool.
The only caveat is if your PST files are largely static archives used for reference, not live files that are constantly changing.
If that were the case then I'd be tempted to manually duplicate the archives (which also gives you an implicit backup) and then use an overlapping retention period/ delayed delete from server to maintain a consistent current message base.
But ultimately you're still "bodging" the system by using POP to achieve this.
However, if it works for you, the purity police aren't going to come knocking and arrest you for crimes against mail protocols.
POP made sense when the act of connecting to a mail server was slow and sometimes even difficult (bloody dial up...) but the real evolution has been in connectivity.
Something like Rackspace hosted email allows large mailboxes, unlimited archiving.
No affiliations, but might be worth a try to see if it will work for you.