When are you going to be there??
As I recall, one of the Excursion bus (
TrapSATur?) tours did Toledo & Segovia in a single full-day tour. They don't run every day of the week, especially when it's off season for Tourists. The concierge at your hotel should be able to set up one of those for ypu with pickup at your hotel or on
c/San Bernado just off the
GranVia.
If you can't do that, my recommendation would be for Toledo. Don't miss the beautiful
Catedral.