Climate change and unsustainable land management practices have resulted in extensive soil degradation, including alteration of soil structure (i.e., aggregate and pore size distributions), loss of soil organic carbon, and reduction of water and nutrient holding capacities. Although soil structure, hydrologic processes, and biogeochemical fluxes are tightly linked, their interaction is often unaccounted for in current ecohydrological, hydrological and terrestrial biosphere models. For more holistic predictions of soil hydrological and biogeochemical cycles, models need to incorporate soil structure and macroporosity dynamics, whether in a natural or agricultural ecosystem. Here, we present a theoretical framework that couples soil hydrologic processes and soil microbial activity to soil organic carbon dynamics through the dynamics of soil structure. In particular, we link the Millennial model for soil carbon dynamics, which explicitly models the formation and breakdown of soil aggregates, to a recent parameterization of the soil water retention and hydraulic conductivity curves and to soil carbon substrate and O2 diffusivities to soil microsites based on soil macroporosity. To illustrate the significance of incorporating the dynamics of soil structure, we apply the framework to a case study in which soil and vegetation recover over time from agricultural practices. The new framework enables more holistic predictions of the effects of climate change and land management practices on coupled soil hydrological and biogeochemical cycles.