I visit Toledo from Madrid last Easter.
We were planning on getting the train but turned up and it was overbooked.
The bus station luckily is around the corner from the main train station so we just headed there
Cant remember whether it was cheaper or not to get the bus, but we arrived in Toledo in a couple of hours.
There was buses every hour (both ways) so we didnt have any problems
The thing I remember mostly was when you bought a ticket you got a seat allocation which I found strange for buses, you also have to remember if you buy a return to go the station office on the way back to get your allocation before they will let you board
We absolutely loved Toledo as well, so what looked like was going to be disaster initially turned out pretty well
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