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I would go for SMT IV personally. Great game though it can be a bit difficult at times (so some grinding might be in order). The story isn't too bad and the game gives you a good amount of stuff to do.

Overclocked is more for you if you favor SRPGs like Fire Emblem and the like.

The tone of both games is pretty dark just like many Atlus games. But I prefer the dialog in SMT IV moreso.
The tone of SMT IV is also pretty far from your standard "anime" fare as well. Sure the characters might say some cliché things from time to time but which game doesn't?