As a WDW Vet, I highly recommend taking a look at
HydroGuy's DLR Guide for WDW Vets. There is a section on rides and that might help you figure out which rides you may want to try riding.
In terms of popularity, I think TSMM is one of the most popular rides in DCA. It doesn't have a FP, so if you want to ride it, you have to stand in line. I agree that it's not necessarily as popular as it is in DHS, in that I haven't seen 2+ hour lines in a while, but 60 to 90 minutes is not uncommon during peak times of the day. The single most popular ride in DCA is going to be RSR. That attraction can have stand-by waits that exceed 2 hours even during non-peak periods of the year. It does have a SRL and FP, so that will help. I would say that Soarin', Screamin', and ToT probably round out the remainder of the long(ish) wait time rides in DCA. A&E and Olaf M&Gs both use a FP/Return Ticket system, so that helps with the lines, but they are also pretty popular.
Over in DL, the most popular rides are probably Peter Pan (just as popular as at MK, but no FP), Space (FP), Indy (FP and SRL), and Matterhorn (SRL). I would also say that Big Thunder (FP), Pirates, and HM (FP sometimes) are popular, but those have lines that move pretty fast. Depending on the weather, Splash can also be pretty popular. Star Tours seems kind of hit-or-miss. Nemo is another ride that can have a very long line (slow loader, no FP or SRL).