The U.S. Environmental Protection Agency (EPA) established the Particulate Matter (PM) Supersites Program to provide key stakeholders (government and private sector) with significantly improved information needed to develop effective and efficient strategies for reducing PM on urban and regional scales. All Supersites projects developed and evaluated methods and instruments, and significant advances have been made and applied within these programs to yield new insights to our understanding of PM accumulation in air as well as improved source-receptor relationships. The tested methods include a variety of continuous and semicontinuous instruments typically with a time resolution of an hour or less. These methods often overcome many of the limitations associated with measuring atmospheric PM mass concentrations by daily filter-based methods (e.g., potential positive or negative sampling artifacts). Semicontinuous coarse and ultrafine mass measurement methods also were developed and evaluated. Other semicontinuous monitors tested measured the major components of PM such as nitrate, sulfate, ammonium, organic and elemental carbon, trace elements, and water content of the aerosol as well as methods for other physical properties of PM, such as number concentration, size distribution, and particle density. Particle mass spectrometers, although unlikely to be used in national routine monitoring networks in the foreseeable future because of their complex technical requirements and cost, are mentioned here because of the wealth of new information they provide on the size-resolved chemical composition of atmospheric particles on a near continuous basis. Particle mass spectrometers likely represent the greatest advancement in PM measurement technology during the last decade. The improvements in time resolution achieved by the reported semicontinuous methods have proven to be especially useful in characterizing ambient PM, and are becoming essential in allowing scientists to investigate sources of particulate pollution and to probe into the dynamics and mechanisms of aerosol formation in the atmosphere.