direct trains and buses from MAD to Toledo?

AFAIK, C1 train to Atocha station, then change to train to Toledo.

Travel time to Toledo is a lot faster by train than by bus, so most foreign visitors use the train. However, a bus has one advantage: The bus station in Toledo is closer to the escalators that take you up to the medieval section of Toledo. I used the Madrid-Toledo bus and had no problem walking and using the escalator. However, with luggage you might prefer to take a taxi, in which case it wouldn't really matter whether you arrived at the Toledo bus station or train station. There are also city buses going up to the historic center. I'm sure you can find one outside either the bus station or the train station. Incidentally, the Toledo train station is very beautiful.

Assuming you decide to travel from Madrid to Toledo by train...

To me, heading to the train station at MAD would be easiest. It will sell you a ticket (or separate tickets if necessary) from MAD to Toledo. You'll need to change trains at Madrid's Atocha Station, which is large. Ask the personnel at the MAD train station to allow a bit of extra time so you don't need to worry about finding the platform for the train to Toledo. Your ticket will be for a specific train to Toledo, with a seat assignment.

Other options are to take the airport bus from MAD to Atocha Station, or a taxi. In both those cases you'll need to buy your Madrid-Toledo ticket at Atocha unless you opt to use the Renfe website or app to do so. Buying your ticket at Atocha is easy, but you have to find the right vending machines--the ones that sell tickets to Toledo--or stand in a line at a staffed counter. Since you're starting from the airport and there's a train station there where you can readily buy your ticket(s), starting there seems much simpler to me.

Although the Metro (subway) goes out to the airport, you have to change lines to get from the airport to Atocha Station, which I'd prefer to avoid with bags in tow. I've used both the train and the airport bus and had no difficulties. I don't know how the costs compare; the train might be less expensive, and it's possible the trip from MAD to Atocha Station is free when you're buying an onward ticket to Toledo. Obviously, the highest-cost option would be a taxi from MAD to Atocha.

Because of the potential sell-out of tickets from Toledo back to Madrid, it would be smart to buy your return train ticket a day or two ahead of time.

If you decide to take a bus from Madrid to Toledo:

Trains between Madrid and Toledo sometimes sell out. That's unlikely to happen to you, but it's not impossible. In that situation, you'd want to take a bus from Madrid to Toledo. The Toledo buses depart from Plaza Eliptica, which has a Metro (subway) stop, but you'd need to change subway lines at Nuevos Ministerios. I believe there's a short, outdoor walk from the Plaza Eliptica Metro station to the bus station. As I recall, the bus station is underground. I'd suggest consulting Google Maps on your cellphone to be sure you're heading in the right direction. I recall being initially puzzled, but there may be good signage now.

I don't think there is any direct (no-change) bus service from the airport to Plaza Eliptica, so the alternative to the Metro ride would probably be a taxi. The distance would be close to 15 miles; I have no idea how much that taxi ride might cost.

While the metro from the airport to Atocha would work, it requires two line changes, so other options are probably faster and more direct.

Our experience was exactly as described by Acraven. Upon arrival we went directly to the Renfe office where we got both tickets to Toledo and our Tarjeta Dorada cards. It is a full service office and not busy. You gotta go through Atocha though but with tickets in hand, no problemo. Brad

AFAIK, C1 train to Atocha station, then change to train to Toledo.

You'll need to change trains at Madrid's Atocha Station, which is large.

FYI, the C1 line now runs only between the airport and Chamartín-Clara Campoamor station. A transfer is required there, such that the complete trip from MAD to Toledo is:

1. Cercanía C1 line from MAD to Chamartín-Clara Campoamor
2. Any Cercanía train that runs from Chamartín to Atocha -- i.e. C2, C3, C4, C7, C8
3. Renfe from Atocha to Toledo

Well, that's annoying.

I believe the only direct route to Atocha now is either Bus or Taxi, Both train and metro require a change, if your flight arrives at Terminal 2/3 (Delta and United) then the train would require getting to terminal 4, which then the Metro would be a better option.