I'd be concerned that a combo tour hitting both the Dali Theatre-Museum in Figueres and the house in Port Lligat wouldn't allow insufficient time at the DT-M. It has been my experience that tour groups go through art museums quite fast, as if they're catering to people who really aren't all that interested in the art. So: How interested are you in Dali? I don't really like Surrealism, but I was surprised to find I really enjoyed the DT-M. I think I spent about 3 hours there. The ticket also covers the nearby jewelry collection, which is fabulous and might require 20-30 minutes. The DT-M does get some bus tours, so it wouldn't be safe to show up without a ticket, expecting to get in immediately; you might or might not. I don't think the place sells out way in advance, but individual time blocks could fill up early.
I believe the visit to the Dali house may be by guided tour. If that's the case, I think your tour would allow you the same time an independent traveler would have there. Incidentally, capacity is very limited at the house; that ticket needs to be purchased way in advance. (Check now for early April!)
Trying to get to both places on your own, on the last day of your trip, could be quite hectic. If I were going to do that, I'd go to Port Lligat first, since it's more awkward to reach: fast train to Figueres Vilafant station, walk/taxi/bus to the other ("Figueres") station, bus from outside that station to Cadaques, walk to Port Lligat. The bus isn't terribly frequent, so I just wouldn't attempt the combo trip independently on my last day in Barcelona.
It would be perfectly reasonable, however, to hop on the train to Figueres and see the Dali Theatre-Museum on your own.
Alternatively, you could take a day trip to historic Girona (closer than Figueres).
Barcelona is a highly walkable city with interesting architecture. You didn't mention seeing the Palau de la Musica Catalana or the Sant Pau modernista site, neither designed by Gaudi but very striking. There are tours of the Palau; English tours may sell out in advance. Many folks opt to attend a performance there and see part of the building that way. The Sant Pau site doesn't require purchase of tickets in advance; you should be able to walk up and get right in.
The city also has multiple art museums, including the large MNAC. The MNAC has a good collection of modernista decorative art, furniture and jewelry, in addition to the expected paintings and sculptures.