A strategy for the on-surface synthesis of silver nanoparticles (AgNPs) on a variety of two-to three-dimensional material surfaces, utilizing polydopamine, an emerging surface modifying agent, is reported in this paper. This material-independent platform for AgNP synthesis is useful for fabricating organic/inorganic hybrid nanomaterials and for preparing substrates for laser desorption-ionization time-of-flight mass spectrometry (LDI-ToF MS).