On the first launch of the application, it builds a local cache of all the .ps, .pdf, and .dvi files available in two locations on your hard disk (/usr/local/teTeX and ~/Library/texmf by default). If the default paths are incorrect for your system, set the correct paths in the Preferences (Paths tab), and choose "Purge Cache Files" from the File menu. When you relaunch TCOBrowser, it will re-cache files according to your locations. These files are then matched with corresponding entries in the XML TeX Catalogue (simply based on filename->package name) if possible, as well as with MiKTeX packages that are available on CTAN.
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