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Static City Twilight shards—these do not respawn.
Rank up social links—Elizabeth will give you a couple of shards every time you establish a new link or rank a link up a few times
Rescue cats—Cats wander into Tartarus about once a month between full moon operations. Elizabeth will tell you "a feline friend has wandered into Tartarus" and tell you which floor it's on. Just get to the floor and walk up to it and it'll hand you some shards (as many as 8)
Tartarus Exploration—You'll see breakable objects in Tartarus with a blue glow. These contain twilight shards.
Dark Floors—After you get the dark floors tutorial, every floor will have a random chance of going dark. Every breakable object that spawns on these floors contains twilight shards, and enemies won't chase you (But the reaper spawns in after 1~2 minutes so be quick)
Even previously-explored floors can turn dark when revisited, so if you're low on twilight shards, just use the teleporter to go to a block you've already explored, and just keep hitting LB to go to the next floor until you get a dark one. Once you're at the top of the block, repeat until you've got enough shards.
These are also affected by the Devil Major Arcana tarot card in shuffle time, so if you've got that, you'll get 2 twilight shards for every object holding twilight shards you break.