Hello! I will be traveling to Madrid and would like to plan a day trip to Toledo on Sunday, March 22. I would like to to get out there earlier than the first train ride which I believe is at 8:50am. (Hoping to be able to attend mass at the cathedral, which I believe starts at 9:45am). Does the bus option not have as many trips to Toledo on a Sunday versus a weekday? I am having trouble seeing or much less booking an early bus ticket. I have used the Asla website, trainline, and renfe websites to see options. Any guidance or information would be greatly appreciated!
I would check the ALSA Bus schedule a little closer to March. You may be searching too far in advance.
Otherwise go to Toledo the night before
I remember an earlier thread or two in which we determined it wasn't safe to spend the night in Toledo if you had a Sunday-morning flight out of MAD, because the trains didn't start running very early. I wouldn't be too surprised if the buses follow a similar pattern, but it's best to wait awhile to see if the schedule gets augmented. I've definitely encountered situations in which the bus schedule wasn't loaded terribly early.
As for the trains, unlike fares for longer-distance trips on the AVEs, the train fare between Madrid and Toledo doesn't vary, so you don't need to worry that you'll be paying a lot more money if you buy your ticket later. It is possible, however, for trains to sell out.
The early morning trains are mainly for commuters, so they don't run on Sat-Sun. The buses may be the same. You won't regret spending a night in Toledo.
Thank you all very much for your input! Decided to go ahead and spend the night in Toledo to be there up and early on Sunday. Can't wait!!