In my opinion, in the world of modern music, notes on the grid don't sound unnatural to me or most people. Notes with rigid velocity do, however. As noted above, having lower velocities on the off-beats sounds better. For a bass part, for example, I might use Find/Change to set everything on a 0 tick to one velocity and everything else to another, lower velocity. After that, however, I would check to see if any off-beat notes needed to be emphasized with full velocity. Bass and drums are easy. An exposed piano part takes time, since some notes are lead notes and some are supporting.
It is very important to know how the instrument is normally played. My favorite true story is about the guy I saw in a music store playing Louie, Louie block chords on an oboe sample and then walking away saying, "That doesn't sound like an oboe."
Also, think about what "natural" means. If it means mistakes or off-beat notes, I wouldn't do it. If it means smooth and flowing, go for it.
For decades we fought to get bass players and drummers to play in time. Now we have sequencers and everyone complains because they play in time. Back to my first point, I think the expression is more critical than the timing.
DISCLAIMER: I am known for making music with instruments that sound too pristine, so if you want to sound like The Band or The Rolling Stones, completely ignore anything I say.