With the aim of mimicking biological machines, in which the delicate arrangement of nanomechanical units lead to the output of specific functions upon the external stimulus, the construction of dual stimuli-responsive rotaxane-branched dendrimers was realized in this study. Starting from a switchable organometallic [2]rotaxane precursor, the employment of a controllable divergent approach allowed for the successful synthesis of a family of rotaxane-branched dendrimers up to the third generation with 21 switchable rotaxane moieties located on each branch. More importantly, upon the addition and removal of dimethylsulfoxide (DMSO) molecule or acetate anion as the external stimulus, the amplified responsiveness of the switchable rotaxane units endowed the resultant rotaxane-branched dendrimers the solvent- or anion-controlled molecular motions, thus leading to the dimension modulation. Therefore, we successfully constructed a family of rotaxane-branched dendrimers with dual stimuli-responsiveness that will be a privileged platform for the construction of dynamic supramolecular materials.