It is impossible to build a cryptographic algorithm using uncomputable problems because you cannot compute them. It would be impossible to execute the encryption. In order to use a problem for encryption, you have to be able to answer it.
For example: you mention the mortal matrix problem, an undecidable problem. It has a "yes" or "no" answer, which is to say that it contains one bit of information. If you had a sufficiently large collection of sets of matrices for which the answer is undecidable, but somehow known to you, you could encrypt a message by exchanging every bit for some representation of a set of matrices with the corresponding answer (eg, "yes" = 1, "no" = 0).
However... it is no less impossible to generate these sets of matrices for you as it is for your 'enemy'. For cases where the answer is easy to work out (such as if all the matrices in a set are already the zero matrix), then you can use them, but you're no better off than using RSA where n = 6. In other words, if you know the answer, then the answer is not really undecidable – the problem may be undecidable in general, but your case is not one of the undecidable cases.
Basically, the way I specified the problem above — "if you had a sufficiently large collection..." — assumes the existence of an oracle – something that magically solves a problem for you. If that oracle really exists and only you and your interlocutor have it, then the whole system just reduces to a one-time pad (an encryption method already known to be unbreakable in theory) with extra steps. In the real world, though, you can't create that oracle because you can't solve the unsolvable problem.