We describe resonance effects in laser desorption–ionization (LDI) of particles that substantially increase the sensitivity and selectivity to metals in single-particle mass spectrometry (SPMS). Within the proposed scenario, resonant light absorption by ablated metal atoms increases their ionization rate within a single laser pulse. By choosing the appropriate laser wavelength, the key micronutrients Fe, Zn and Mn can be detected on individual aerosol particles with considerably improved efficiency. These ionization enhancements for metals apply to natural dust and anthropogenic aerosols, both important sources of bioavailable metals to marine environments. Transferring the results into applications, we show that the spectrum of our KrF-excimer laser is in resonance with a major absorption line of iron atoms. To estimate the impact of resonant LDI on the metal detection efficiency in SPMS applications, we performed a field experiment on ambient air with two alternately firing excimer lasers of different wavelengths. Herein, resonant LDI with the KrF-excimer laser (248.3 nm) revealed iron signatures for many more particles of the same aerosol ensemble compared to the more common ArF-excimer laser line of 193.3 nm (nonresonant LDI of iron). Many of the particles that showed iron contents upon resonant LDI were mixtures of sea salt and organic carbon. For nonresonant ionization, iron was exclusively detected in particles with a soot contribution. This suggests that resonant LDI allows a more universal and secure metal detection in SPMS. Moreover, our field study indicates relevant atmospheric iron transport by mixed organic particles, a pathway that might be underestimated in SPMS measurements based on nonresonant LDI. Our findings show a way to improve the detection and source attribution capabilities of SPMS for particle-bound metals, a health-relevant aerosol component and an important source of micronutrients to the surface oceans affecting marine primary productivity.