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That being said, If you are on Act 2, The combat shells in the courageous training rooms drops U-materials.
In addition to that, yes, the shells are the most reliable way to farm U-materials, because their U-material is a 100% drop and you still get those drops even if you flunk the training objectives. If you just want a handful of them, using the Ymir hot springs and blasting them down with S-crafts is the quickest way to do so. Particularly if you have the Domination Quartz.
If you want to farm larger quantities of them, it's best to wait until you're about to cross the point-of-no-return, at which point you get a piece of quartz that doubles the power of the first offensive art you cast. (you should already have a quartz that increases physical/magical damage if the enemy's lower level than you) With those pieces of quartz equipped, as well as some EP Cutting quartzes, you can challenge the level 3 training and use a combination of Chrono Burst and Sol Eruption/Lost Eden to nuke the shells the moment your turn comes up and because your EP gets recharged after every battle (unlike your CP), you can keep doing that over and over.
I had gone through all of the "DLC" U-material before I was finished with the first Act and still probably farmed between 300 and 400 from the lvl 3 melee combat shells. In addition to what I had gotten from random mob drops. By the finale MOST of the quartz I had equiped were rare or super rare with the only normals I had being basic Attack/action/impeed 2/3's I also had 4 abyss shadows 4 evergreens 5 passionate rogues and 2 still blues most of which were one that I upgraded from pedulums which requires between 25 to 40 U material each.