Launchbox doesnt even do what you are asking to romfiles, its true it only imports working games but you still have the not imported games on your system, unless you manually delete them like you seem to of done. As i said though Launchbox doesnt do anything with CHD files, it doesnt even know they exist, so has no way of deleting what you dont need. Also there is a major flaw in what you are proposing, so you delete all roms and CHD's for games that dont currently work, then next month MAME add 10 new working games, well you are out of luck then as you have deleted those now working games, where as people who just use our importer to import working games will still have those in there collection.
Also as a last thing, what you are doing relies on having a full non-merged set, which as you say is around 110GB, thats why most people dont even use a non-merged set, they use a merged or split set, that are around 60GB instead. You can not just delete roms from those sets as other completely different games may be using files in completely unrelated roms.
As for the CHD's its very easy to get a list of working games that need a CHD from MAME itself and delete what doesnt work/or what you dont care to play. Personally my CHD collection is about 50GB only.