I hope you weren't thinking you'd only have to read one book...
Learning the .NET API is key. For that, I would recommend:
* read CLR via C#, Second Edition, by Richter
I taught myself C# and my first year of code was rather hideous until I started spending time on Design Patterns. The following books are good:
* Patterns of Enterprise Application Architecture (Hardcover) by Martin Fowler
* Head First Object-Oriented Analysis and Design A Brain Friendly Guide to OOA&D By Brett McLaughlin, Gary Pollice, David West
* Design Patterns C# (Hardcover) by Steven John Metsker (Author)
For web, I would recommend the following ASP.NET books:
* Programming Microsoft ASP.NET 2.0 Applications: Advanced Topics by Dino Esposito (Paperback - Mar 15, 2006)
* Programming Microsoft ASP.NET 2.0 Core Reference by Dino Esposito (Paperback - Nov 30, 2005)
You definitely need to do code so I would start some sort of project for someone, like a non-profit, in .NET. Unless you have a preference I would start with web as there are more jobs there. I think.
.NET 3.0 is here and there are new ways you can structure your programs, particularly for a winform application. I would really learn that as well and try to do something interesting there.
Also, C# isn't the only language thats hiring. You might want to consider Java or other alternatives to the windows world. Windows keeps me employed, but if I was to start my own company, the startup costs are too high for a windows environment.