There are many highlights along the valley, these are my favorites (Some are just outside the valley)
Purmamarca actually is located off the main road in the valley. It is on the road towards Attacama desert in chile via the amazing Paso de Jama. This makes it a great stop on the way to and from Chile. The town is very small and was the most ‘touristy’ town in the area. Best for a day trip, check out the main square which is full of markets stalls. Another site is the Cerro de los Siete Colores (The hill of seven colours). It has a unique color range that is the product of a complex geological history including marine sediments, lake and river movements elevated with the movement of the tectonic plates.
Amboro National Park
I found Tilcara to be the best place to stay as it has alot of hostel options and great restaurants (more than the other towns). Traces of human habitation in the area date back more than 10,000 years, making it one of the oldest continuously inhabited settlements of Argentina. There is also an amazing day hike to ‘Devils Throat’, that has great views of the area, waterfalls, and a water aqua-duct.
Las Cuevas Waterfall