With the already limited time to visit Madrid and Barcelona ,along with a desire to do day trips from these base cities, I'd take the high speed train between these cities. There's just not enough time to squeeze in a long drive and day of sightseeing between Barcelona and Madrid.

Nobody has mentioned the Reina Sofia in Madrid, Picasso's Guernica and more, also Dali.
Also Retiro Park is a nice stop if you have time.

Toledo is a nice town to walk, but our friends took the little train and got some great photo ops as well.

Danon- a day in the car is hard on the waist, but I agree, it also seems a waste of time : )

Sorry for the spelling


English is not my first language....it is my fifth.

Toledo is a must and I would go for Girona from Barcelona or maybe Figueres if yoou like Dali.
http://theartichokeadventures.blogspot.com.es/

Danon you are doing very well then, a lot of us with English as a first language have trouble spelling....

Thank you so much for all your suggestions. This is our first time in Spain and there is so..... much to do! I plan to look up everything and make a list of all I want to do and I guess what I get done, I get done and the rest will be left for another time.

Again Thanks!! You were all so very helpful!

Do NOT take the slow train from Madrid to Barcelona - that's nearly six hours and kills one of your very few days.

Do NOT drive - both cities have good public transportation and a 6-8 hour drive from Madrid to Barcelona will, again, kill one of your very few days of travel.

DO be careful - Barcelona is a haven for pickpockets and petty thievery. Just be aware. No one tried anything against me and we had two perpetual distractions (daughter, son, both under 5) with us at all times in Barcelona.

Oh, and if you like modern art (e.g., you don't think the phrase is an oxymoron or only 1/2 accurate), go here: http://www.articketbcn.org/en/index. Big savings.