Cycling research at the operational behavioral level is limited, mainly because of the lack of empirical data. To overcome this data shortage, we performed a controlled, large-scale cycling experiment in the Netherlands. In this paper we describe the methodology for setting up and implementing such an experiment, from the motivation of its design using a conceptual model describing cyclist behavior to adjustments that were required during the experiment. The main contribution of this paper is, therefore, to be used as a guide in future experimental data collections. Moreover, we present the characteristics of the participants and their bicycles, and provide a qualitative description of phenomena observed during the experiment. Finally, we elaborate on the potential that the collected dataset holds for future research into understanding and modeling operational cycling behavior.