I would get off I-25 and use highway 64 through Cimarron, Eagle Nest, Angel Fire and Taos. The circle around through Red River is also nice. See the Rio Grand Gorge outside Taos. Kit Carson and his family are buried in Taos. Lots of colorful homes there, too. From Taos, take "the High Road" to Espanola. This goes through scenic country, as well as small villages and pueblos. In Chimayo is the Santuario de Chimayo, very historic and scenic. Also a great restaurant in Chimayo (Rancho de Chimayo).
You can day-trip north on 84 to Abiquiu, Georgia O'Keefe's Ghost Ranch, Echo Canyon, etc, etc. To the SW are Los Alamos, Jemez Valley (caldera, actually) Bandelier NM, etc, etc.
Santa Fe is special, lots of churches and other historic buildings. Loretta's Chapel is a must see. The national cemetery appeals to me. Day trip to visit the Zia Pueblo, descendants of the Anasazi.
Spend some time with Google to round out your itinerary.