Since the count is not calculated until the report is printed (or displayed in preview mode), it is not possible to sort by the count because Access doesn't know what it is ahead of time. The recordset is always sorted before the report step.
The solution is to create a query that includes only the break fields and a Count(*) function. Then join this query to your existing query, pulling in the count field. You will now be able to sort by the count field because you have calculated it ahead of time.
I'm going to make up an example because your question gives no clue as to what your application is. Assume you have a report that lists order summaries for customer.
countquery:
Select CustomerID, Count(*) AS CountOfOrders
From OrderTable
Group By CustomerID;
yourPresentquery:
Select CustomerID, OrderID, OrderDate, OrderTotal
From OrderTable;
newversionofyourpresentquery:
Select O.CustomerID, O.OrderID, O.OrderDate, O.OrderTotal, Q.CountOfOrders
From OrderTotal AS O Inner Join countquery AS Q On O.CustomerID = Q.CustomerID
Order by Q.CountOfOrders, O.CustomerID, O.OrderID;