One of the problems you have with natural ingredients is the sheer volume you have to use to cause death. Buttercups are toxic, but you'd have to eat an entire field to kill yourself (not to make you sick, but to actually kill you). There aren't that many plants with toxin so concentrated that it can kill you in small amounts. Yew seeds and leaves are one (
http://www.nlm.nih.gov/medlineplus/ency/article/002877.htm) and the mortal dose is quite small (
http://www.botanical-online.com/alcaloidestejoangles.htm) and it does grow in Europe. It causes slow heart rate and can cause death in 30 minutes.
Another one is Oleander (
http://www.nlm.nih.gov/medlineplus/ency/article/002884.htm). It's a decorative plant that might be used in gardens, like foxglove.
A third natural option is castor bean, the source of ricin. It's a common decorative plant in gardens.
Someone here suggested injecting air--the problem here is that you need to inject about a liter of air to have it actually stop the heart.
Acetylcholine is an injectable that kills, and is naturally present in the body. It actually degrades after death, so if the medical examiner doesn't think to check for it really quickly, it's gone.
Another option is insulin. It's a commonly available injectable drug that an overdose is rarely detected, especially if the body takes a little while to be discovered. People test for blood sugar, not for the insulin itself. A body that takes several hours or a day to be discovered continues to chew up blood sugar, so it's ordinarily low in a postmortem blood sample of this kind.