Atomic force microscopy (AFM) is a stylus‐based technique that uses sub‐nanonewton force sensitivity to image surfaces at sub‐nanometer resolution. As a surface‐sensitive tool, AFM is ideal for investigating the properties and local morphology of surface‐grafted supramolecules and (bio)polymers, which play important roles in mediating interfacial processes ranging from tribology to colloidal stability and biology. Moreover, the versatility of AFM to operate in diverse environments (i.e., air, liquid, or vacuum) adds to its appeal in comparison to other surface methods. Given its capability for high‐resolution imaging, force measurements, and nanomechanical manipulation, AFM is directly applicable to studies of stimuli‐responsive polymers, biomaterials, and polymeric nanostructures.