For a fairly accomplished C# developer, Expert F# is the best book to learn F#.
The book is elegant, fun & practical.
The examples are genuinely interesting. My favorite ones are in chapter 9, Introducing Language-Oriented Programming: probabilistic workflows, schema compilation by reflecting on types, and using F# quotations for error estimation.
The book will really help you master techniques specific to F# and functional programming in general. For example, there's a section called "Using Continuations to Avoid Stack Overflows". Like the rest of the book, it's very clear and insightful.
(One issue is that the book was written before the F# CTP, so some of the examples might not work with the latest release. However, it is usually rather straightforward to update the samples.)
So, yes. Get this book and have fun :)