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This series consists primarily of tornado observations and eyewitness accounts solicited from the general public via newspaper advertisements in areas where tornadoes and severe storms frequently occur. They are filed using the original labeling system employed by Dr. Vonnegut, where the date and place of the observation as well as a brief statement on the phenomena is used to identify the observation. Accounts of severe storms found in multiple publications, biblical references, and other historical observations are also present.

Series 10 contains files on a wide variety of subjects; people, articles, topics in science, and other topics of interest to Dr. Vonnegut throughout his career.

Series 8 documents the work that Dr. Vonnegut did while employed at SUNY Albany. During his time at SUNY Albany, Dr. Vonnegut taught classes, served on committees, attended conferences, and continued his research concerning weather, lightning, and clouds. Much of the research that Dr. Vonnegut did while at SUNY Albany was done as part of government research projects. Most notable was his work on Project Themis which was conducted by the United States Air Force. The project's main focus was on the modification and structure of clouds and fog but also investigated other areas of research such as raindrop dynamics and atmospheric electrical phenomena

This series documents the Project Cirrus program, a weather modification initiative undertaken by GE along with the United States Signal Corps, Office of Naval Research, and the United States Air Force, with general oversight handled by the Department of Defense. As part of the effort, Dr. Vonnegut discovered that AgI, Silver Iodide, was a superior nucleation agent. This discovery significantly influenced the science of artificial precipitation and this method came to be adopted as the chief means of "rain making".

Series 4 documents Dr. Vonnegut's work with the New Mexico Institute of Mining and Technology (NMIMT) in Socorro, New Mexico. While both were employed at Arthur D. Little, he and fellow scientist Charles Moore were invited to conduct thunderstorm research at Mt. Withington, eventually becoming part of the Langmuir Laboratory for Atmospheric Research in Socorro. Moore stayed at NMIMT, and Dr. Vonnegut moved on to the State University of New York at Albany; though their collaborative research continued for the entirety of each other's career.

This series contains records for professional conferences and meetings arranged and/or attended by Dr. Vonnegut as well as project proposals, reports, correspondence, travel arrangements, conference programs, meeting agendas, registrations and other conference-related items, press release, and records on the classes he taught. Additionally, this series includes papers written by others that Dr. Vonnegut found interesting or pertinent to his research.

Series 7 consists of Dr. Vonnegut's published and unpublished articles, letters to the editor, papers, reviews, reports, and book/encyclopedia chapters. Many files contain the research and data discussed within the work, as well as correspondence with the editor(s) of publications where work was submitted.

Series 6 contains Dr. Vonnegut's general interest and research files, as well as the inventions that he worked on throughout his career. Topics include: lightning, ball lightning, lightning strikes and the effect on aircraft, volcanic activity and storms on Mt. St. Helens and Surtsey, thunderstorm electrification, and weather-related instruments.

Dr. Vonnegut's audio/visual series consists of materials related to his research and presentations as well as the work done by some of his colleagues, especially Duncan Blanchard and Vincent Schaefer. The formats included in this series are VHS, cassette, reel to reel, ½" open reel, 8 mm film, super 8 film, and 16 mm film. Visual materials come in both color and black and white formats. Items have been titled based on Dr. Vonnegut's own identification system. Any audio or video which Dr. Vonnegut did not name are listed as Untitled.

While employed at Arthur D. Little, Dr. Vonnegut built upon his research in atmospheric science. The majority of his work focused on electrification of clouds, thunderstorms, and the behavior of lightning, he also looked at behaviors of gases but on a much smaller scale. Besides pursuing his own research, Dr. Vonnegut worked on a number of advisory projects for the United States government. These projects focused on the relationship between aircrafts and lightning. The main focus was on how aircrafts detect and avoid lightning when flying in a storm.