Quick reviews of the highlights....
Castle Works Ultimate - a very nice modular castle.

Not (yet) available in a TLX format, but excellent for, well, castles.
Himmelveil Canals - canals in a TLX format. Also contains docks, pilings, some nifty walls with inlets and outlets, some spewing water, others not, and a canal lock. Best used with another TLX set, since it is otherwise missing some necessary pieces. Speaking of which....

Looks like a dwarf to me....
Lost Halls - a modular kit for building a lost dwarven stronghold. For some reason I have always pictured dwarfs building canals, this set goes wonderfully well with Canals, especially since the faces around the water outlets and inlets have a definitely dwarven look to them.

These two are well purchased as a pair. My favorite for this installment.
Shellendrak Manor - a modular haunted house kit. I have not used it much, aside from a 3D Clue board I built a few years ago as a Christmas present. Not TLX compatible, but nice, and very versatile for building modern or Victorian houses.
Harbor Master - a non modular kit for building a Victorian style harbor master's office/home. It can also be used for a train station, and in fact has seen a lot more use as such when in my games.
Mayhem Marina - a modular, nonTLX harbor for modern games, and includes a tugboat. Docks, buildings, and a few, umm oddities (what
is that thing on the hook?).
Mars Station - a small frontier town on Mars? Definitely SF, but somehow it feels a bit like the old West.
The Auld Grump