We report for the first time the construction of mechanoresponsive and redox-active metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) by anchoring ferrocene (Fc) pendants as mechanophores in the pore wall. This work outlines a simple, general, and low-cost route to tailor MOFs and COFs by a Fc unit for mechanoresponsive nature, the release of Fe ions, redox behavior, and modulation of the skeleton charge together.