The Sort method takes a delegate called Comparison<T>. You're trying to pass in a Func<int, int, bool>, which is itself a delegate. There is no conversion between the delegate Func<int, int, bool> and the delegate Comparison<T>.
You can, however, use a lambda expression.
items.Sort((a, b) => a.DateModified.CompareTo(b.DateModified));
Indeed, you use this very lambda expression and pass it into the Func<int, int, bool> constructor*. However, there is no need. A lambda expression can be converted into any delegate whos signature matches - that is (a, b) => a.DateModified.CompareTo(b.DateModified) can be assigned to something typed Func<int, int, int> or something typed Comparison<T>. In this case we pass it in to something which expects a Comparison<T>.
* With one minor adjustment. Sort expectes an integer as a return type. Negative values indicate less than, 0 indicates equal, and positive values indicate greater than.