AbstractMechanoenzymology is an emerging field in which mechanical mixing is used to sustain enzymatic reactions in low‐solvent or solvent‐free mixtures. Many enzymes have been reported that thrive under such conditions. Considering the central role of biopolymers and synthetic polymers in our society, this minireview highlights the use of mechanoenzymology for the synthesis or depolymerization of oligomeric or polymeric materials. In contrast to traditional in‐solution reactions, solvent‐free mechanoenzymology has the advantages of avoiding solubility issues, proceeding in a minimal volume, and reducing solvent waste while potentially improving the reaction efficiency and accessing new reactivity. It is expected that this strategy will continue to gain popularity and find more applications.