This study uses in situ experimental investigation techniques to probe the synergistic effects of aqueous phase viscoelasticity and reduced interfacial tension on nonwetting phase displacement efficiency in natural porous media. Specifically, it examines the efficacy of viscoelastic surfactant (VES) solutions in enhancing oil recovery and investigates the pore-scale displacement mechanisms and VES−oil interactions. To this end, we first performed an extensive rheological characterization to select two VES solutions from multiple CTAB/NaNO 3 (CTN) and Cocobetaine/SDS/ NaCl (CSN) mixtures. The selected aqueous solutions were then used in unsteady-state imbibition experiments conducted on miniature, water-wet Prairie Shell carbonate core samples. The experiments were performed utilizing a high-pressure, high-temperature two-phase core-flooding apparatus integrated with a high-resolution X-ray imaging system to acquire pore-scale fluid occupancy maps during the displacements. The results indicate that the injection of the selected CSN and CTN solutions into the carbonate samples under capillary-dominated flow regimes boosts the oil recovery by 12 and 2%, respectively, compared to those of the base waterflood. The VES solutions lowered the oil−water interfacial tension and exerted significant shear forces at the entrance of pores. The shear forces could exceed the threshold surface free energy required to deform oil globules, and consequently, large oil clusters were fragmented into smaller blobs and eventually produced from the pore space. The higher oil recovery by CSN flooding was attributed to its stronger viscoelastic properties. The VES injection under the viscous-dominated flow regime intensified the frequency of oil globule fragmentation. As a result, residual oil saturation values were sharply reduced in the rock samples from 44 to 55% during the capillary-dominated flows to approximately 8%. The above-mentioned observations were also verified using morphological analysis of residual oil clusters. The impacts of VES flooding on the pore-scale oil configuration and the fragmentation of large oil clusters were particularly evident at higher VES flow rates.