Aluminum alloy castings are becoming commonplace for critical applications in the automotive and aerospace industries where materials failure is not an option. In order to meet such property demands, tight control over the cleanliness of the melt (mitigation of solid particle inclusions) and microstructure must be achieved. In order to control cleanliness, it must first be well defined and measured. Very few techniques exist in industry that can quantitatively measure inclusion levels in-situ. Laser-induced breakdown spectroscopy (LIBS) is presented as a promising technique to quantify solid particles, desired or undesired, in aluminum melts. By performing LIBS with subsequent statistical analysis on liquid aluminum with varying concentrations of Al2O3, AlB2, TiB2, and SiC particles, calibration curves relating particle concentration and elemental intensity were drawn. Through metallography and automated electron microscopy, it was found that inclusions less than 10 um in size could be detected with LIBS. Concentrations down to at least one part-per-million could be detected and accurately measured, allowing for LIBS to be use as a tool for complete, real-time melt cognition.