LAUSR

Abstract Microfabrication of complex double emulsion droplets with controlled substructures, which resemble biological cells, is an important but a highly challenging subject. Here, a new approach is proposed based on laser‐induced injection of water nanodroplets into a liquid crystal (LC) drop. In contrast to the conventional top‐down microfluidic fabrication, this method employs a series of bottom‐up strategies such as nanodroplet injection, spontaneous and assisted coalescence, elastically driven actuation, and self‐assembly. Each step is controlled precisely by adjusting the laser beam, interfacial tension, and its gradients, surface anchoring, and elasticity of the LC. Whispering gallery mode illumination is used to monitor the injection of droplets. A broad spectrum of double emulsions with a predesigned hierarchical architecture is fabricated and reconfigured by temperature, laser‐induced coalescence, and injection. The proposed bottom‐up method to produce customized microemulsions that are responsive to environmental cues can be used in the development of drug delivery systems, biosensors, and functional soft matter microstructures.