A robust strategy is explored to graft poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) brushes on two-dimensional vanadium carbide (V2C) materials through self-initiated photografting and photopolymerization (SIPGP). CO2 and temperature dual-responsive properties of PDMAEMA allow this hybrid to be used as a smart system for tuning the transmittance and conductivity of V2C.