Could be an option, yes.

Well, if you look at their collector coins, Luxembourg does have quite a few interesting series and issues. But those are all fairly expensive ...
As for the designs of the commemorative €2 coins, blame the European Union, and blame the (or some) euro area countries. On one hand we have the "rule" that the ring of a euro coin, including the commems, has to display the Stars of Europe as they appear on the flag. While I fully agree with and support the idea of using the stars - we already have them on the common sides. Why not arrange them in a circle there? Then the other side could in its entirety be used for the country specific design.
This way we would also have more space for "mandatory" elements. A small portrait of Henri could then appear somewhere on the obverse of such a commemorative €2 coin. Would not look "tiny" but would leave enough room for the main design so to say.
Then again, some member states seem to prefer those somewhat monotonous designs. It is Luxembourg's decision to show the head of state of each coin, just as it is Ireland's decision to use the harp and nothing else (except for the country name and year) on their circulation coins ...
Christian