Linq To Objects - (C#) Creating A Dictionary From An Existing List Without Looping?

I don't know if this is doable, maybe with Linq, but I have a List(Of MyType):

Public Class MyType
Property key As Char
Property description As String
End Class

And I want to create a Dictionary(Of Char, MyType) using the key field as the dictionary keys and the values in the List as the dictionary values, with something like:

New Dictionary(Of Char, MyType)(??)

Even if this is doable, internally it will loop through all the List items, I guess?