The fastest way from Faro, Algarve, Portugal to Toledo or Madrid is as marked on the following google map:
http://bit.ly/91QV37
Transit Times: 7 hours.
I have driven this route several times. It is toll-free motorway all the way apart from near Madrid. Fuel in Spain is cheaper than in Portugal. The road is also newer and better than the Seville - Cordoba - Madrid route. Speeds of 100/120 km per hour can be maintained on most of the route except around cities.
To summarise:
Faro to Seville - A22/A49
Seville to Merida - A66
Merida to Toledo/Madrid - A5
The A66 runs through some beautiful countryside.
Have a great trip
