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For the chipped stone "Gothic" blocks, I'd recommend either the Dragon's Inn #51 (if you're planning to make houses and town buildings), the Wizard's Tower #50 (if you intend to do castles), or the Dungeon Builder #45 (for modular dungeon sections). With either of the latter two, you'll also need a floor tile mold, since they don't include a floor tile. The Inn mold at least gives you one full 1" square floor tile (not much, but better than none), but a dedicated floor mold is still a big help.

For Fieldstone, the FS Wall mold #70 is the only logical choice. Either the Flagstone Floor mold #260 or the Cracked Floor Tiles #203 are strongly recommended for flooring, since #70 only includes a half-tile and a quarter-tile, and the half-tile is only semi-usable for flooring because it's designed to be placed vertically.

The problem with the Tomb mold as a starter isn't so much the difficulty as the fact that it doesn't give you any "basic blocks". It's great for trim, but first you'll need something to hang that trim onto.

The Gothic Bridge #53 is "usable" as a starter mold, but the shortage of basic blocks means you need to cast it a ridiculous number of times to build anything more than "trinkets". Same goes for the FS Bridge.

The "usual" starters are the three I listed above, and it all depends on your focus as to which of the three to get. You can get the Prison Tower, for instance, and have a couple basic blocks and a floor tile along with all the arches and trim, but it gets frustrating to cast and cast and cast, with very little progress to show for it. Many of these make good "second" molds.