The mountain villages around here have kept their simplicity and traditional character, notably Anidri to the northeast, with a frescoed 14th century church. Towards Soughia, on a pretty rough road (8km) is Azogyres, a very green place with a stream and a small historical museum (open Sat and Sun 9am-2pm) which is quite interesting and which deals with the period of the Turkish occupation. .At the bottom of this village, next to the chapel of Aghios Pateres is a very rare evergreen plane tree, and the chapel has a carved iconostasis which is the work of a local craftsman. Above this village is the cave of Soure said to have been temporarily occupied by the 'Holy Fathers' (pateres) who had returned from Egypt after the return to Byzantine rule in Crete. There is a metal stairway and rock steps descending into the cave. Taking a flashlight/torch is a good idea if you want to go any distance, though.
Travelling northwest from Paleohora (with your own transport and a willingness to drive some unpaved stretches) there is a wonderful route along the valley of the Pelekaniotikos River, that passes some beautiful villages, Voutas, Kamatera, Arhondhiko, Strovles and Mili, after which the road meets the road south to Elafonisi.