No, there was really only one crossover. In "Birthright, Part 1" from TNG's season 6, Dr. Bashir helps Data and Geordi with something while Picard, Crusher, and Worf are visiting DS9. There isn't much to the visit besides Picard and Crusher talking about the station and Worf having a significant conversation with an alien who isn't even part of DS9's cast (guest star James Cromwell). Oh, and there's also a scene between Picard and Sisko in the DS9 pilot and an episode in TNG during which Quark talks to Riker on the viewscreen.
They really should have had more crossovers, maybe even on the big screen. Would have much rather seen the TNG crew involved in the significant events happening on DS9 around the time of "Star Trek: Insurrection", instead of the nothing story that the movie ended up with. Also, it sucks that in their one and only scene together, Sisko implies that he blames Picard for everyone Locutus killed, as he can barely conceal his (unfair) contempt for the man as a result. I wish there'd been a follow-up where he forgave Picard, because it just made Sisko look like a tool.
Anyway, to answer your question, it's not like "Buffy: The Vampire Slayer" and "Angel" where there's a huge advantage to watching the two series with chronologies in sync. In those two series, episodes pick up right where an episode for the other series left off. Nothing so direct happens between DS9 and TNG. On the other hand, my personal opinion is that the first two seasons of DS9 are really shaky and you're better off getting started as soon as possible...the sooner you get to the much improved season 3 and the really good stuff of seasons 4 to 7, the better.












