The most “green” type of hairspray is the kind you make yourself at home.
Here is a recipe for making hairspray that involves natural ingredients, the main one being lemons:
This website has a bunch of organic hairsprays to choose from: http://www.nextag.com/organic-hairspray/stores-html. Most of them are non-aerosol, and pump versions are better for the ozone. If you are going to buy hairspray at the grocery store, check for bottles that are recyclable in your city.
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