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The Carbon journal is pleased to introduce a themed collection of recent articles in the area of computational carbon nanoscience. This virtual special issue was assembled from previously published Carbon articles by Guest Editors Quan Wang and Behrouz Arash, and can be accessed as a set in the special issue section of the journal website homepage: www.journals.elsevier.com/carbon. The article below by our guest editors serves as an introduction to this virtual special issue, and also a commentary on the growing role of computation as a tool to understand the synthesis and properties of carbon nanoforms and their behavior in composite materials.