Barcelona to Granada and more - Train, Bus, Flight?

Barcelona-Granada by airlines Vueling or Spanair...usually the cheapest and most effective. The earlier you book, the better price you will get, but watch luggage allowances and charges, and check-in procedures. The Spanish rail company, RENFE, offers an overnight train. With bookings available up to 62 days in advance, you may be able to get a two-berth second class sleeper (very comfortable) for about 67 Euro per person. The site is in Spanish, but navigable....www.renfe.es .
For Granada-Barcelona, either train or bus. The time is about the same (3 hours) and the prices are close, but the buses run much more frequently....they are comfortable. You can check bus schedules and fares at www.movelia.es
Sevilla-Madrid, definitely the high speed train.,..2.5 hours. The RENFE website is again the place to go as soon as you are able, and get fares up to 60% off...second class fares from about 32 Euro per person...second class is very comfortable.
Madrid-Toledo...same thing....AVE high speed train, half an hour for less than 10 Euro. There's no web special for booking in advance. But since this is a popular train, you may still want to book ahead to ensure seats on the train(s) you want.
All train tickets can be printed at home...they'll show up at the end of the booking process as a pdf file...save a copy to your computer.

My wife and I took the night train from Barcelona to Granada in 2005 and it worked great. A travel agent can get you set up, that's what we did.

Seville to Madrid on the high speed train, same trip also worked great. This was in late September and we did not book ahead. The train was really full so in retrospect perhaps not booking ahead could have turned out badly.

For Toledo there are also buses, so I would not worry too much about it.

Granada to Seville we took the train and bought the tickets when we arrived at the station. Slow train, about three hours, but we got there.

Wow - thanks SO SO much. I really appreciate all of the help!