DON'T whatever you do... decide to walk from the coach station or the train station up into Toledo. From the train station there is an easily found bus stop; from the bus station there isn't. When you get off the bus or the train find the taxi rank asap. Ask the driver for Plaza Zocodover. At the station the rank is directly outside; at the bus station it is up the moving stairs, left though glass door, immediately right and keep straight on to the edge of the building. There are not all that many taxis... I say this because the walk up the hill to the city, especially in summer, is awful and when you get to the top is the time to start exploring. You can always walk back down! Cost of taxi 6€ - well worth it! (2013)
I recommend using buses rather than trains for getting between towns and cities in Spain. They are both cheaper and quicker than the trains which tend to take indirect routes and are unreliable. The best routes to use the train for is between Barcelona to Madrid (2 hours) and Madrid to Seville (2 hours). These routes are covered by the AVE - an express train which covers the large distances between both points in a couple of hours rather than the usual 6-7 hours which the much slower regional 'express' trains take.
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