The fabrication and properties of pH‐responsive colloidal particles are reported, which change shape rapidly (less than 200 ms), nearly independent of the diffusion of the pH altering species that trigger their actuation, and far more rapid than their Brownian motion. These particles are mechanically bistable, as revealed by their hysteretic shape response. Finite element analysis (FEA) shows that mechanical hysteresis and bistability derives from the colloids' spherical curvature. Mechanical characterization of the bilayered polymers comprising the colloidal particles shows that viscoelastic relaxation plays a non‐negligible role in limiting the shape switching rate; however, energy landscapes obtained from FEA simulations suggest that by tuning the elastic moduli and thicknesses of the constituent polymer layers, microparticles of the size shown here may be fabricated to actuate on timescales as fast as 1 μs.