Definitely do the Maderas Volcano hike. It takes about 8 hours and is strenuous, but when you climb over the rim of the crater and walk down inside to the lake, there are few experiences as breathtaking.
It is like a step back in time to some secret Jurassic place where you wouldn't be surprised to see a dinosaur saunter out of the woods. It also has a very cool and powerful feeling to it that is difficult to describe and you see a variety of landscapes from volcanic rock fields to dense jungle. You just need to go!
I would suggest a guide. There are a myriad of trails and navigating them can be tricky. People have become lost and died. The volcano looks smaller than it actually is and the whole hike is about 12km because of the long lead up to the actual crater edge. Guides can be hired at any local hotel, but check out Finca Santa Cruz at the crossroads leading to Belgue and Merida. It will cost you between $10-$15 per person.
Bring at least 3 liters of water, lunch, a couple snacks and a decent pair of shoes. I did it in Converse and my feet and knees were not happy about it the next day. Oh and you will sweat - a lot, but a tall Tona beer at the end of the day never tasted so good :)
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