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I would split it along Roman Lines
I like this idea in general, though there are some problems with the North in your set up
If the diocese of Caledonia is everything North of hadrian's wall, that puts the Bishops of Rhinnydd and Gododdin under a Dal Riatan Archbishop. Rhionydd basically only exists because Dal Riata is propping them up, so they won't complain too much, but the Gododdins won't like it one bit. The Picts and Scoti are basically their mortal foes, they won't stand for having one overthem.
And yet, if the Caledonian boarder is whatever North of Antonine's wall, it makes the archbishopric of Lindkolon HUGE, when compared to their nominal head in Gloucester.

So to solve this, the area between the walls will be the diocese of Valentia, with the Archbishop in Dineidyn.
Map time! Archbishoprics are marked with a yellow dot
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