The main road is south from Vrysses , which winds up on the Plateau of Askifou (about half-way to the south coast. This was the road where the evacuation of Allied troops happened after defeat by the Germans in the Battle of Crete in May, 1941. It is also the scene of the massacre of Turkish armies by the Cretans both at the beginning of the War of Independence in 1821, and in 1866 after the events at Arkhadhi Monastery (see Rethymnon) during the same struggle.
Villages on the plateau include Amoudhari, from which hikes in several directions are possible, one of them an arduous walk via Kali Lakki of 18km southwest to Anopoli (on the south coast just west of Hora Sfakion) Without explicit directions, this walk might be a bad idea, though. Other walks both east and west are easier, including one to the village of Atsigonia. Be aware in general that the Greek sense of time and distance is usually different from that of foreign visitors, and that details in trekking guides might be more reliable than the estimates of villagers, which often turn out to be a fraction of the reality (much to the chagrin of the unititated).
From Anopoli, should you venture this hike, you can get to the Aradhena gorge to the west in about an hour. There are old paths that descend down one side and up the other, inland a bit. The village across the gorge is abandoned, but there's a Byzantine church there with some frescoes. There's a car road to, with a bridge across the gorge, which ends another 5km to the west at Aghios Ioannis. The coast trail (near Aghios Pavlos) will get you to Aghia Roumeli in about five hours (17km), though one might allow extra time.
There's another hike from Loutro up the gorge and over the Anopoli, but the gorge is quite steep and only the very fit should tackle it. It is, however, a beautiful place.