Ecological sustainability is the defining challenge of our time. Here we suggest a methodological approach that could help to investigate how environmental behavior (transport behavior, energy consumption, food consumption, goods consumption, wasting) dilemmas can be overcome on an individual level in real life by using smartphones to collect daily behavioral data in a field-experimental setup. Previous related studies are reviewed and we discuss how the boundaries of what can be done with smartphones for data collection and experimental purposes can be pushed further to allow for complex behavioral studies. Results from a pilot study are presented to discuss the feasibility and potential of this approach. The pilot shows that studying social dilemma behavior via smartphones is feasible and has potential value as a behavioral intervention tool.