Your options are pretty limited with just the DS and PS2. The best options available are FF X-2, FF XII on the PS2 and FF III, FF IV on the DS.
FF X-2 is a pretty good companion piece to FF X. As a game its nowhere near as good but is worth a playthrough and it finishes off the story of Yuna and Tidus pretty well(depending on which ending you unlock).Most of the characters are poorly fleshed out. Also has a mission structure and active time battles. Brings back job classes as well. Worth getting for anything less than the equivalent of fifteen euros.
FF XII is a game which has received a lot of flak but when it boils down to it its one of the better games in the series. The story is absolutely epic, the voice acting is second to none, there is a huge world to explore with plenty of side missions, graphically the best game of the previous generation and the combat is fluid. It lacks that old FF magic though and Vaan has to be one of the worst protagonists in the whole series. Probably the best option.
FF IV is nothing short of a retro classic, the same applies to III. What they lack for in modern game mechanics they make up for with old school charm. The combat is perfectly balanced and the stories are not half bad. I would choose IV over III given the choice though.
If you have the money and patience to find FF VII, VIII and IX on the original PS1 that would be the best option. These are the holy trinity of the series in my opinion and as close to perfect as games can get. These games are perfectly balanced as well as brilliantly paced. The stories are all great. If I had to put them in order though I would put VII first, then VIII and then IX.
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