Hydrological and geochemical monitoring are key components of site characterization and CO2 plume monitoring for a pilot test to inject CO2 into a brine-bearing sand of the fluvial-deltaic Frio formation in the upper Texas Gulf Coast. In situ, injected CO2 forms a supercritical phase that has gas-like properties (low density and viscosity) compared to the surrounding brine, while some CO2 dissolves in the brine. The pilot test employs one injection well and one monitor well, with continuous pressure and flow-rate monitoring in both wells, and continuous surface fluid sampling and periodic down-hole fluid sampling from the monitor well. Pre-injection site-characterization includes pump tests with pressure-transient analysis to estimate single-phase flow properties, establish hydraulic connectivity between the wells, determine appropriate boundary conditions, and analyze ambient phase conditions within the formation. Additionally, a pre-injection tracer test furnishes estimates of kinematic porosity and the geometry of flow paths between injection and monitor wells under single-phase conditions. Pre-injection geochemical sampling provides a baseline for subsequent geochemical monitoring and helps determine the optimal tracers to accompany CO2 injection. During CO2 injection, hydrological monitoring enables estimation of two-phase flow properties and helps track the movement of the injected CO2 plume, while geochemical sampling provides direct evidence of the arrival of CO2 and tracers at the monitor well. Furthermore, CO2-charged water acts as a weak acid, and reacts to some extent with the minerals in the aquifer, producing a distinct chemical signature in the water collected at the monitor well. Comparison of breakthrough curves for the single-phase tracer test and the CO2 (and its accompanying tracers) illuminates two-phase flow processes between the supercritical CO2 and native brine, an area of current uncertainty that must be better understood to effectively sequester CO2 in saline aquifers.