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If this Toll-Free number is one of the company numbers and not assigned to an extension, there is no option to block all calls for this number because it will block from all other company numbers you have.

Is it possible, then, to remove the toll free number from the system entirely? As in, would deleting that number from the account have any sort of knock-on effect to the rest of the phone system? As mentioned, we don't use the number, don't want to use the number, and all we get on that line is spam.

You need to contact your Account Manager for this. It depends on your plan subscription. Another option would be to change the number completely.

Thank you so much for the advice - I'll do what you suggested!

You're welcome!