It is generally appreciated that the mechanical behavior of granular media depends fundamentally on the interaction of the constituent particles, and that the validity of numerical models of granular media would be greatly improved with knowledge of the grain-scale mechanics. However, most supporting experimental work has been conducted on highly idealized materials, and a limited amount of information exists on grain-scale force–displacement relationships for naturally occurring materials. To address this shortcoming, we are conducting a program that integrates laboratory experiments on grains of naturally occurring aggregate with the discrete element modeling method, with the goal of relating the grain-scale physical and mechanical properties of granular media to bulk behavior. The paper describes the equipment and methods that have been developed to conduct close-loop controlled, grain-scale experiments under monotonic and cyclic loading conditions, and presents results from an initial set of experiments on unbonded grains. The implications of the grain-scale results to the discrete element model are discussed. Discussions center on the applicability of a physically based approach to the mechanics of granular media in general. In light of future exploration missions and the resulting need to predict the mechanical properties of lunar and planetary regoliths, the paper examines the potential usefulness of our physically based approach to the problem of predicting the behavior of the types of materials found in those environments.