Safeguarding water resources for society and ecosystems requires a comprehensive understanding of hydrological fluxes within the Critical Zone, Earth's living skin where the atmosphere, hydrosphere, biosphere, and lithosphere meet. For decades, tracer‐aided mixing models have been used to track water flow paths through the Critical Zone, mapping the journey of water particles from atmospheric moisture to groundwater. Recent advances in novel tracer measurements and modeling methodologies offer new insights into hydrological partitioning within the Critical Zone, enabling improved quantification of water fluxes across scales ranging from microscopic to macroscopic. Advanced tracer‐aided modeling approaches enable more rigorous testing of assumptions and improved quantification of uncertainties. In this review, we (a) summarize state‐of‐the‐art tracer and modeling techniques, with an emphasis on stable water isotope tracers, (b) synthesize insights emerging from new approaches, and (c) highlight opportunities to apply these methods in interdisciplinary Critical Zone research.