Monitoring the migration of sequestered in deep heterogeneous reservoirs is inherently difficult. Geophysical methods have been successfully used, but flow conditions are only indirectly linked to the measured properties. Besides geophysical methods, pressure tomography (PT) is proposed as an alternative method to depict the structure of deep saline formations for sequestration and to continuously delineate plumes. In contrast to more established geophysical measurements, pressure transients are directly related to flow properties, which allows for the estimation of permeability. We investigate the influence of aquifer heterogeneity on PT performance, and we compare the PT results to crosshole seismic tomography (ST). Multilevel fluid injections and high-frequency P-wave pulses are induced in a simulated deep borehole, and the recorded signals at another well are processed by a traveltime inversion scheme. The reservoir structure is inferred by clustering the inverted hydraulic diffusivity prior to injection, and the plume distribution is determined by clustering the tomograms of the inverted mixed-phase diffusivity difference and P-wave velocity difference. The clustered structures are then used for zonal calibration to acquire the saturation within the plumes. Modeling results indicate that PT provides clearer structural information on the -free aquifer due to its direct linkage to permeability. However, the plume depicted by PT can be ambiguous, whereas ST is less sensitive to the prevailing heterogeneity of permeability at postinjection and can thus image the plume more clearly. PT and ST can be complementary to each other through the joint clustering to improve plume shape identification and estimation of spatial saturation.