A high-throughput method was proposed to screen coating fillers with both good corrosion-sensing and inhibition performances. SiO2 nanoparticles loaded with different percentages of phenanthroline (Phen) and 1-hexadecyl-3-methylimidazolium chloride (HDMIC) were prepared (Ph-HD@SN) using a multi-channel synthesis instrument. The corrosion-sensing ability of different Ph-HD@SN to detect Fe2+ ions can be determined by spectrophotometric method within 30 s. The corrosion inhibition effect of Ph-HD@SN was evaluated by visual assessment and quantification of iron dissolution from carbon steel in NaCl solutions containing different nanoparticles. The optimized Ph-HD@SN was incorporated into epoxy coating to achieve the corrosion-sensing and self-healing properties.