Land Surface Models (LSMs) are prospective starting points to develop a global hyper-resolution model of the terrestrial water, energy and biogeochemical cycles. However, there are some fundamental limitations of LSMs related to how meaningfully hydrological fluxes and stores are represented. A diagnostic approach to model evaluation is taken here that exploits hydrological expert knowledge to detect LSM inadequacies through consideration of the major behavioural functions of a hydrological system: overall water balance, vertical water redistribution in the unsaturated zone, temporal water redistribution and spatial water redistribution over the catchment's groundwater and surface water systems. Three types of information are utilised to improve the model's hydrology: (a) observations, (b) information about expected response from regionalised data, and (c) information from an independent physics-based model. The study considers the JULES (Joint UK Land Environmental Simulator) LSM applied to a deep-groundwater chalk catchment in the UK. The diagnosed hydrological limitations and the proposed ways to address them are indicative of the challenges faced while transitioning to a global high resolution model of the water cycle.