color changes to adapt to different environments by tuning the spacing of guanine nanocrystals; [12] salmon can find their way by using magnetite NPs on their forehead in response to Earth's magnetic field. [13,14] Inspired by nature, researchers and engineers have devoted intensive efforts to control the aggregation of "smart" NPs for constructing superstructures by regulating external stimuli. Generally, these "smart" NPs are obtained through two main approaches. One is to assemble functional molecules to NPs (nanogels, [15] proteins, [16] etc.) by covalent/noncovalent interactions. However, little attention has been paid on their aggregation caused by external stimuli. The other most popular method is to decorate functional ligands (small molecules, supermolecules, polymers, etc.) onto the surfaces of NPs (inorganic metal, metal oxide, silica, etc.). These ligands can provide a variety of interactions (e.g., hydrophobic interactions, hydrogen bonding, electrostatic interactions, and host-guest interactions) to regulate NP aggregation under different external stimuli. The combination of smart NPs and external stimuli provides an amazing and promising route to create functional materials or devices with highly tunable unique properties.For many decades, stimuli-responsive NP aggregation at micro or macroscale has aroused great interest and broad explorations for its potential applications in biomedical engineering, [17] robot technology, [18] and energy conversion. [19] Since Mirkin et al. reported a DNA-based method to assemble NPs into macroscopic aggregates by thermal variation in 1996, [20] many intelligent multiscale assembly of smart NPs from nano/ microscopic aggregates to macroscopic materials have been spatio-temporally realized in a remote way by various external stimuli such as temperature, pH, light, electric, and magnetic fields. Several typical NP superstructures have been created at nano/microscale, such as disordered aggregates, [21] ordered superlattices, [22] structural droplets, [23] and colloidosomes. [24] To obtain large macroscopic materials is still a great challenge, notwithstanding a few successful examples, centimeterscale-ordered bulk solids [25] and switchable liquid-solid bulk materials. [26] Some excellent reviews have summarized the NP assembly methods and strategies, such as evaporation-induced NP assembly, [27,28] polymer-guided NP assembly, [29,30] biomoleculemediated NP assembly, [31,32] etc. In this review, we focus on the recent advances of stimuli-responsive NP aggregation systems that have been developed to construct some typical functional Stimuli-responsive nanoparticle (NP) aggregation plays an increasingly important role in regulating NP assembly into microscopic superstructures, macroscopic 2D, and 3D functional materials. Diverse external stimuli are widely used to adjust the aggregation of responsive NPs, such as light, temperature, pH, electric, and magnetic fields. Many unique structures based on responsive NPs are constructed including disordered aggregates, order...