You can't really do that, as you have two strings per row and you can;'t put two strings into a single string unless you concatenate them.
Probably what you want to do is closer to this:
string[] str = new string[4];
str[0] = "USD";
str[1] = "60.1";
str[2] = "INR";
str[3] = "0.165";
string[][] anotherarray = new string[str.Length / 2][];
for (int i = 0, x = 0; i < str.Length && x < anotherarray.Length; i += 2, x++)
{
anotherarray[x] = new string[2];
anotherarray[x][0] = str[i + 0];
anotherarray[x][1] = str[i + 1];
}