Canter
In my opinion, I believe that these places can be done as a day trip although others may disagree. I know that on my next trip back to Spain I will be going back to Toledo for a second look and am even giving "some" consideration to staying there at least 1 night, but then the question arises as to what to take and what to leave behind in Madrid.
Others have indicated that the Bus is a better alternative than the train. I haven't personally used the Bus Service in Spain so I can't comment. Maybe some others can. I believe that there has been some postings on this matter so if you do a search here something may come up.
David