Inverse design of structural colours in polymeric films with crystallization-induced reversible thermochromism

Precisely controlling structural colours in polymeric materials remains a major challenge, with current approaches often relying on trial-and-error synthesis. Here, we develop a colour design model, enabling inverse design of structural colours in bottlebrush block copolymers (BBCPs). The model can quantitatively link BBCP molecular structures to macroscopic colours through the integration of a strong segregation self-consistent field theory model with a multilayer optical framework. We first validate its predictive capability by synthesising and assembling BBCPs with varied chain architectures to produce a full colour spectrum, and then demonstrate its generalisability to other BBCP chemistries. In addition, we observe reversible, nonlinear thermochromism in systems combining a crystalisable block with a soft, low–glass transition temperature segment, while similar BBCPs lacking this pairing show no such response. Our work establishes a predictive platform for designing structurally coloured, thermoresponsive polymeric materials and advances the rational engineering of photonic soft matter.