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Abstract We present a versatile platform for fabricating two‐photon excitable carbon dot‐based nanocomposite thin films by harnessing the structural versatility of polymer brushes in combination with electron‐beam lithography (EBL). This approach enables the precise spatial organization of carbon dots (CDs) at the nanoscale, facilitating dynamic modulation of their photoluminescent properties in response to environmental stimuli. Three model systems were examined, incorporating pH‐ and thermally responsive polymers, functionalized through covalent and dynamic covalent bonding strategies. By leveraging the spatial control afforded by nanostructured polymer brushes, we achieved precise tuning of optical properties while mitigating aggregation‐induced quenching, a longstanding challenge in solid‐state CD applications. In addition to the advances in controlling optical properties, this work highlights the potential of polymer brush systems to function as optically active, reprogrammable surfaces. The resulting nanoscale‐engineered materials exhibit highly responsive, reconfigurable photonic behavior, offering a scalable pathway for integrating advanced optical interfaces into microchip technologies, biosensing platforms, and multiplexed diagnostic systems. The fusion of polymer brushes, carbon dots, and advanced lithographic techniques marks a substantial advancement in the development of functional materials with nanoscale precision and stimuli‐responsive properties.