Mass spectrometry has been applied to the characterization of organoaluminum compounds in work that dates back to the introduction of the first commercial instruments. As new ionization methods and associated instrumentation were developed, they have been applied to more difficult analyses so as to characterize the compounds of increasingly higher molecular weight, low volatility and ionic organoaluminum compounds. In thifs chapter, practical advice for performing these analyses, and choice of ionization method(s) to be applied is provided, as well as a representative survey of the various mass spectrometric techniques that have been applied to analysis of organoaluminum compounds.