Safe and efficient storage of CO2 in saline aquifers requires mobility control to prevent CO2 from accumulation and rapid spreading at the formation top below the caprock. In the past, we have demonstrated the effectiveness of two engineered olefinic-based oligomers for viscosification of sc-CO2 and the significant improvement in residual trapping of sc-CO2 in brine-saturated homogeneous sandstone cores. The objective of this work is to examine the sweep efficiency and residual brine saturation in the layered cores by effective viscosification with two engineered molecules, providing the implications for CO2 trapping in layered porous media by effective viscosification. In neat CO2 injection, the CO2channels through the high permeability layer, causing rapid breakthrough and high residual brine saturation. This results in an inefficient process for CO2 storage in saline aquifers. In viscosified CO2 injection, we observe significant improvements in crossflow at the interface between the two-permeability layer, partly due to the mobility control and residual brine saturation reduction. In comparison to the neat CO2 injection, the synergistic effect of the mobility control and increases in interfacial elasticity by injection of vis-CO2 results in delay in breakthrough by a factor of 2 and about 95% higher brine production. Compared to our previous work on displacement experiments in homogeneous sandstone core, there is a more significant reduction of residual brine saturation in layered cores by viscosified CO2 injection. Increases in injection rate is also demonstrated to improve the CO2 storage in layered cores. Both the CO2 viscosification and increases in injection rate may promote the injection pressure to overcome the capillary entry pressure, leading to CO2 displacement of brine in the low-permeability layer. CT-imaging data advances understanding of boundary conditions, brine production, and local residual brine saturation in layered cores.