We report a general click chemistry approach for the layer-by-layer assembly of ultrathin, polymer films on particles and the subsequent formation of polymer click capsules (CCs). Poly(acrylic acid) copolymers, synthesized with a minor component of either alkyne (PAA-Alk) or azide (PAA-Az) functionality, were alternately assembled on silica particles. The (PAA-Az/PAA-Alk)-coated particles were subsequently functionalized by exploiting the free alkyne click moieties present in the film upon exposure to an azide-modified rhodamine dye. Further, PAA CCs, obtained following removal of the silica particle template, were shown to exhibit pH-responsive behavior. This was demonstrated by reversible size changes of the CCs upon cycling between basic and acidic solutions. Polymer CCs are anticipated to find applications in various fields, including drug delivery and sensing.