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, ordered superlattices, structural droplets, colloidosomes, and bulk solids. In this review, the strategies for NP aggregation by external stimuli, and their recent progress ranging from nanoscale aggregates, microscale superstructures to macroscale bulk materials along the length scales as well as their applications are summarized. The future opportunities and challenges for designing functional materials through NP aggregation at different length scales are also discussed.