After spending much time searching for a bike rental place (I could not use the Villo city bike rental since I don't have a chip in my credit card), I managed to find the De Woudpoort (Brusselsesteenweg 700, 3090 Overijse), a very friendly establishment occupying an old forest rangers station on the northern end of the forest. For 12€ you get a day rental (10AM-6PM) with either a city or mountain bike. To be honest the city bike works just fine and has added storage space. The De Woudpoort also has a wide range of local beers, cheeses, and pastries not to mention a decent forest exhibit and info center.
As for the forest itself it was quite nice to get outside of the cities and touristy stuff and escape into wildness. The trails are well kept although a little confusing to navigate, I found myself going down pedestrian and equestrian trails from time to time as the bike paths seemed to disappear or merge. But in about 1.5 hours ride from De Woudpoort I found myself scurrying through Waterloo on the way to the memorial which is undergoing a major renovation at the moment.
Definitely a must do if you're looking to kill a day and just want some fresh, clean air!
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