Better choice from Madrid Airport to Toledo, Bus from Plaza Eliptico or Train from Atocha Station?

The airport is northeast of the city while Plaza Eliptica is southwest of it.

Could you take the metro to the plaza to catch the bus, yes, but Atocha is closer and the trains run frequently.

Trains leave about once per hour to Toledo. I would not book ahead either, but that is me. It is often mentioned that trains can sell out, but usually that are the trains coming back to Madrid at the end of the day, sometimes in the morning as the Daytrippers head out. mid-day when you will be there, I think it is unlikely.

For the Bus station, the Metro is your best option, get on the line servicing the airport, get off at Nuevos Ministerios, change to Line 6, there is a Metro stop right in the Plaza.

Time wise? Depending on timing, the Bus/Train has a faster travel time, Metro/Bus is Cheaper. You can buy a fully changeable round trip bus ticket ahead for less than 10 euro, it does not appear you need to buy for a specific bus, just get on.

Thanks, frequency of the trains is probably my biggest question. Sound like the train option is easier and better.

I've only been through Atocha a couple times. I'm used to buying a ticket from a machine. I have to steer our two friends, who arrive on a different flight and have never been to Europe, to Toledo also. It seems like there are multiple ticket offices as well as a travel agency in Atocha. I think getting on the Expres bus is easy enough. How would you explain, as simply as possible, how to buy tickets, and catch the train, to Toledo from Atocha? I'm thinking steering them toward the travel agent.

They should be able to go to the ticket counter and get tickets, language should not be an issue, though there could be a line. The machines are pretty straight forward to use, but a bit slow in that you have to enter in passenger info and passport number. Not sure if the travel agent would even bother with a Toledo ticket, they are a help for multiple destinations or if there are station changes.

At Atocha, you will need to find the area that the Toledo trains leave from, they will direct you, but track number may not be listed until 10 minutes or so before departure.

There is a newer level for the fast trains not sure if the Toledo trains leave from there, or one of the other levels. In either case, they will need to go through security (quick check your ticket, toss your bag on a belt for an x-ray machine) before proceeding to the train.

There is a staffed train station at the airport where you can buy a ticket to Toledo that will cover your ride to Atocha Station. The folks at the airport train station will sell you an appropriately-time ticket to Toledo. Unless there's a problem with the trains running into town from the airport, that's what I'd opt to do if I was heading right to Toledo. Atocha can be a bit confusing, it's true, but it would be nice not to have to start with finding the right ticket machines for the trip to Toledo.

There's nothing wrong with hopping on a bus at the airport to get to Atocha, either. I've done that without difficulty, but I think it's easier in your situation just to use trains.

While the Metro can also get you from the airport to Atocha, I think two transfers are required, and that's a pain.

Thanks for your replies