Lanthanide-doped upconversion nanoparticle (UCNP)-based nanocomposites can address the intrinsic limitations associated with UCNPs and bestow new functions on UCNPs, which can facilitate the development and application of UCNPs. However, the fabrication of UCNP-based composites typically suffers from complex operations, long-drawn-out procedures, and even loss or damage of UCNPs. Herein, we report a tandem fabrication strategy for the preparation of UCNP-based nanocomposites, in which protons, confined in the non-aqueous polar solvent, can produce ligand-free UCNPs for the direct fabrication of a composite without further treatment. Our studies show that the confined protons can be generated by diverse materials and can yield different types of ligand-free nanomaterials for desired composites. This versatile strategy enables a simple but scalable fabrication of UCNP-based nanocomposites, and can be extended to other nanomaterial-based composites. These findings should provide a platform for constructing multifunctional UCNP-based materials, and benefit potential applications of UCNPs in varied fields.