Compartmentalization is a powerful concept to integrate multiscale components with diverse functionalities into miniature architectures. Inspired by evolution-optimized cell compartments, synthetic core-shell capsules enable storage of actives and on-demand delivery of programmed functions, driving scientific progress across various fields including adaptive materials, sustainable electronics, soft robotics, and precision medicine. To simultaneously maximize structural stability and environmental sensitivity, which are the two most critical characteristics dictating performance, diverse nanoparticles are incorporated into microcapsules with a dense shell and a liquid core. Recent studies have revealed that these nano-additives not only enhance the intrinsic properties of capsules including mechanical robustness, optical behaviors, and thermal conductivity, but also empower dynamic features such as triggered release, deformable structures, and fueled mobility. In this review, the physicochemical principles that govern nanoparticle assembly during microencapsulation are examined in detail and the architecture-controlled functionalities are outlined. Through the analysis of how each primary method implants nanoparticles into microcapsules, their distinct spatial organizations within the core-shell structures are highlighted. Following a detailed discussion of the specialized functions enabled by specific nanoparticles, the vision of the required fundamental insights and experimental studies for this class of microcarriers to fulfill its potential are sketched.
Keywords: bio‐inspired nanocomposites; compartmentalization; core–shell microcapsules; multifunctional materials; multiscale structures; nanoparticle assembly; smart microcarriers.
© 2024 The Authors. Small published by Wiley‐VCH GmbH.