A novel Au dimer-based colorimetric sensor is reported that consists of Au dimers to a chitosan hydrogel film. It utilizes the ultrasensitively gap-dependent properties of plasmonic coupling (PC) peak shift, which is associated with the dynamical tuning of the interparticle gap of the Au dimer driven by the volume swelling of the chitosan hydrogel film. The interparticle gap and PC peak shift of the Au dimer can be precisely and extensively controlled through the pH-driven volume change of chitosan hydrogel film. This colorimetric sensor exhibits a high optical sensitivity and stability, and it works in a completely reversible manner at high pH values. Importantly, the sensitivity of the composite film can be tuned by controlling the crosslinking time of the composite film, and thus leading to a wide dynamic tuning sensitive range for different applications. This presented strategy paves a way to achieve the construction of high-quality colorimetric sensors with ultrahigh sensitivity, stability and wide dynamic tuning sensitive range.