Proper way to initialize a C# dictionary with values?

I can't reproduce this issue in a simple .NET 4.0 console application:

static class Program
{
    static void Main(string[] args)
    {
        var myDict = new Dictionary<string, string>
        {
            { "key1", "value1" },
            { "key2", "value2" }
        };

        Console.ReadKey();
    }
}

Can you try to reproduce it in a simple Console application and go from there? It seems likely that you're targeting .NET 2.0 (which doesn't support it) or client profile framework, rather than a version of .NET that supports initialization syntax.

With C# 6.0, you can create a dictionary in following way:

var dict = new Dictionary<string, int>
{
    ["one"] = 1,
    ["two"] = 2,
    ["three"] = 3
};

It even works with custom types.

You can initialize a Dictionary (and other collections) inline. Each member is contained with braces:

Dictionary<int, StudentName> students = new Dictionary<int, StudentName>
{
    { 111, new StudentName { FirstName = "Sachin", LastName = "Karnik", ID = 211 } },
    { 112, new StudentName { FirstName = "Dina", LastName = "Salimzianova", ID = 317 } },
    { 113, new StudentName { FirstName = "Andy", LastName = "Ruth", ID = 198 } }
};

See Microsoft Docs for details.