Conventional CO2 EOR techniques based on microscale chemicals have limited efficiency in tight reservoirs because the micro-nanopores of these reservoirs impede their injectivity and propagation in porous media. This work elucidated a novel well-defined silica nanohybrids named DMA-NPs with the distinct CO2 switchability for enhancing CO2 flooding in tight reservoirs. DMA-NPs densely encapsulated with a CO2-functional moiety of dimethylamine was synthesized by sequential surface modification and amidation reaction. The proof-to-concept for the CO2-switchable nanohybrids was studied by TEM, TGA, SEM, 1H NMR, FT-IR, DLS, rheological measurements and core flooding tests. The results indicated that DMA-NPs underwent reversibly physical transition, from stable colloidal particles with hydrodynamic diameter of 62nm to a relevant viscoelastic fluid, by repeatedly bubbling CO2 or introducing air to remove CO2. Moreover, DMA-NPs dispersion whose viscosity was close to water, could preferentially flow through dominant porous media. When the dispersion met with the displacement front of CO2, these stable colloidal particles self-assembled into a relevant viscoelastic fluid which reduced CO2 mobility and diverted CO2 into a lower permeable zone, and thus more than 30% of original oil in place bypassed by the initial CO2 displacement was recovered.