Yes, you can. But you can argue if it's very pretty...
Int64[] aValues = new Int64[] { 1, 2, 3, 4, 5, 6 };
var result = aValues
.Select( ( x, y ) => new KeyValuePair<Int64, Int32>( x, y ) )
.GroupBy( x => x.Value / 2 )
.Select( x => x.Select( y => y.Key ).ToList() ).ToList();
How it works:
Select x and y from the original collection, where x is the actual value and y is the index of it in the given collection. Then group by integer devision of the index and the desired grouping length ( in this example 2 ).
Grouping by integer devision will round up to the lower - so 0 / 2 = 0, 1 / 2 = 0, etc. which will give us the needed grouping category value. This is what we are grouping against here.
For result select only the values grouped in lists and return them as a collection of lists.