If the work-piece allows I sometimes start the process with the chuck standing vertically on the bench; using the marker-rings and a rule to centre the work as close as I can.
Then with the jaws nipped up, mount the chuck plus work for final adjustments.
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How fussy I am with the latter depends on the purpose.
If needing full concentricity with an existing feature such as a machined periphery or bore then I use a DTI.
If not critical, using the tip of a tool almost touching the periphery as a pointer may be close enough: the machining takes care of the important areas.
For very close accuracy on an item already machined all over but difficult to test by indicator, such as for modifying the bore of a gear, then one approach is to use a “nest” turned in a sacrificial disc secured to the faceplate. Conversely, mount the bors on a mandrel protruding through the chuck or faceplate.
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One snag with setting larger 4-jaw chucks is that some have concave jaw faces, so as you push the work across one diameter it tries to climb the hills on the other. I am not sure of the best way here, as it seems one pair of jaws is fighting the other.
Incidentally there is an old alternative for very awkwardly-shaped work; and that is the faceplate with face-plate dogs. I have not seen much mention of these at all in modern literature, but they would seem potentially useful fittings when used appropriately. They effectively turn the faceplate into an multi-jaw chuck, but may be safer used in conjunction with intervening clamps.
On which, why not faceplates with six slots? There are many items with 3, 6 or 12 bolts-holes etc in them!