IMO, building good levels with the rough-edged tilesets is
harder; not nessecerially impossible though. Especially in the lower ranks, where aesthetics are arguably more important than challenge factor, the rough tilesets can be quite useful. However, when it comes to hard levels, they're definitely easier to make with the smooth sets - definitely in my experience, the majority of my hard levels (apart from those that are so-called "Nintendo hard" rather than genuine hard; for example Mental 25), either use the smooth graphic sets, or if they use a rough tileset, they tend to use the smooth
pieces of them. The most obvious symptom of this is the rarity of Sky levels in my higher difficulty ranks, as that consists solely of rough (or at least curved) edges.
That's not to say I don't have any genuine-difficulty levels using them; some that come to mind are:
LPI: Psycho 18
LPII: Genius 1, Genius 4, Genius 18 (NeoLemmix version obviously)
LPII Bonus Pack: Flight 6, Rush 4
LPIII: Fierce 8. Probably my hardest rough-edge tileset level of all time. There's others, but they're dwarfed by this one.
LPIII Bonus Pack: The final levels of all three gimmick ranks (two of which are using the Sky set, amazingly; the third one is Martian)
Holiday LP: Arctic 5, Arctic 6
LP Omega: Mental 8, Mental 12, Mental 15, Mental 24