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GIS and computational tools like ArcGIS are best learned in a comprehensive manner during a for-credit course. But if you want to go it alone, or brush up, these are some good websites.
GIS Primer (PDF document)
This is a somewhat old, but still useful introduction to GIS book by David J. Buckley. He allows visitors to download the entire full-text PDF (about 5 MB).
Getting Started with GIS
Free course from ESRI. Requires a (free) ESRI account, but a good starting place.
New to GIS?
Introductory pages from the Wiki GIS online encyclopedia.