The field of micro-optics (e.g., lenses and mirrors) has been of considerable interest over the past decade as photonic applications attempt to keep up with the trend of device miniaturization. Microlenses in particular have been applied to fields, such as telecommunications, image analysis, [1,2] and photolithography. [3±5] Microlenses and microlens arrays are well known and can be accomplished by a number of routes, such as photolithography, [3±6] photothermal patterning, [7] photopolymerization/photo-curing, [8±10] and polymeric particle self-assembly/melting. [11,12] These systems have been studied in detail but often have the shortcoming of requiring multiple fabrication steps. A self-assembly approach, in which the microlens precursors are synthesized by traditional solution polymerization routes and are then directly assembled on a substrate would be extremely beneficial with respect to the speed of fabrication and the ultimate size limitations of such arrays.In the approach explored here, thermoresponsive poly[Nisopropylacrylamide-co-(acrylic acid)] (pNIPAm-co-AAc) hydrogel nanoparticles (microgels) were assembled on an aminopropyltrimethoxysilane (APTMS) functionalized glass substrate through common electrostatic interactions. The amine groups present on the substrate are available for electrostatic binding to the acrylic acid (AAc) modified microgels. Because the pNIPAm-co-AAc microgels are mechanically soft, it is possible for the attractive forces between the substrate and the microgel to cause the microgel to deform upon attachment and subsequent drying to produce a microgel decorated substrate where the particles are deformed in an anisotropic fashion. These pNIPAm-co-AAc microgels are also environmentally responsive, [13±15] so it is possible that the microgel curvature could be controlled by modulating the environment they are deposited under, i.e., temperature, pH, and solvent quality. Such particles could also be used for dynamically tunable lensing structures, where the stimuli-sensitive polymer is used to tune the size, focal length, and/or refractive index of the lens. Finally, it may be possible to control the optical properties, responsivity, and focusing power of such lenses by controlling the optical/mechanical properties of the polymers used to make the microgels, the ªsoftnessº and hence deformability of the microgels, and the surface chemistry used to immobilize the lenses.Microgels that are approximately 2 lm in diameter in their water-swollen state were used to fabricate microlenses. A differential image contrast (DIC) microscope image of the microgels adsorbed to a glass substrate is shown in Figure 1a. Microgels were adsorbed to an APTMS functionalized glass substrate by exposing the glass substrate to a 10 vol.-% aqueous microgel solution for approximately 1 h. The substrate was then rinsed with deionized H 2 O and air dried for approximately one day prior to imaging. Because these microgels are soft/deformable materials it should be the case that when the microgel dries on a ...