I've not done this specifically to a 100-4 cylinder head, but I have modified cast iron heads for Triumphs and Austin Minis. In each case, the head was not the only modification, so its hard to tell how much benefit there was...
Also, the key is not just to better align the ports, but to remove material around the valve guides and in the intake "bowl" under the valve. Port matching will not yield much of a result on its own. Also important is combustion chamber shape, particularly around the valves. I will say the cast iron is significantly harder to work than aluminum, and therefore more time consuming, but its also more forgiving than aluminum. It will require a valve job after modification, so that's a good opportunity for some larger valves and a 3 angle hardened seat for unleaded. While you're at it, a cheap way to raise compression is to "mill" the head face to shrink the combustion chamber size. I once milled over an 1/8 inch off of a Mini head to raise compression and found good results.
In general, though I can't speak to the AH 100 head specifically, Cast iron British cylinder heads respond well to port and combustion chamber modification especially when combined with CR and a cam change.
* Don't attempt this though without knowing what you are doing-- it is easy to ruin a head with too much grinding. The David Vizard engine modification book is a good resource.