At a glance, it does seem to make sense. After all, the prefix -un is commonly used to convey the meaning of something which is opposite of X, where X is a particular verb. Words such as uncommon, untruthful, unflattering or unclear are examples.
The interesting thing about the word, unborrowed, though, is that it is not as commonly used as we might think it is. In fact, after checking with a number of dictionaries such as the Merriam Webster, Oxford Advanced Learner's Dictionary, Longman Web Dictionary, First U.S. Learner's Dictionary etc, this word couldn't be found. There was no entry for this word. Well, Merriam Webster has it in the unabridged version though, which I have no access to.
BUT I managed to find an entry in the OED! :D
unborrowed, ppl. a.
Not borrowed or taken on loan; esp. fig., not adopted from another, native, inherent, original. (Common from c 1700.)
1638 G. DANIEL Eclog i. 256 Oh doe not thinke but She may be as faire In nature's bounties, with vnborrwed haire.
Looking at the quotations for the word unborrowed, the examples are all rather old. The latest is 1871 and that is quite long ago. In addition, the use of the word seems to be in contexts which are significantly different.
Therefore, using unborrowed to refer to books which have not been loaned or checked out from the library yet would be a rather unusual use of the word. Unborrowed doesn't even seem to be in use today, or maybe rarely. Entering the word on Google UK and filtering only UK sites produced only 2000+ search results which is somewhat of an indication of how seldom this word is used.
I really wonder then, how did such a word become such a commonly used word in the local context, especially in libraries? I suspect there was some assumption about the usage of the prefix -un and its productivity. People probably thought it attaching it to borrow would produce the meaning of something which has not been borrowed. What they did not realise is that the result unborrowed is a little different, since unborrowed looks like a really natural construction with a straightforward meaning.
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