This work describes the use of fast-evaporating micro-droplets to finely disperse nanoparticles (NPs) in a polymer matrix for the fabrication of nanocomposites. Agglomeration of particles is a key obstacle for broad applications of nanocomposites. The classical approach to ensure the dispersibility of NPs is to modify the surface chemistry of NPs with ligands. The surface properties of NPs are inevitably altered, however. To overcome the trade-off between dispersibility and surface-functionality of NPs, we develop a new approach by dispersing NPs in a volatile solvent, followed by mixing with uncured polymer precursors to form micro-droplet emulsions. Most of these micro-droplets contain no more than one NP per drop, and they evaporate rapidly to prevent the agglomeration of NPs during the polymer curing process. As a proof of concept, we demonstrate the design and fabrication of TiO2 NP@PDMS nanocomposites for solar fuel generation reactions with high photocatalytic efficiency and recyclability arising from the fine dispersion of TiO2. Our simple method eliminates the need for surface functionalization of NPs. Our approach is applicable to prepare nanocomposites comprising a wide range of polymers embedded with NPs of different composition, sizes, and shapes. It has the potential for creating nanocomposites with novel functions.