Hello @ImperialWalker ,
There is no great way to get from this point to where you want to go. There is not enough information about form here, and it would not be possible to flatten one of the polygroups without also deforming the adjacent polygroups in non-planar fashion. Note that ZBrush does not support NGons, so it would not be possible to collapse a 6 point shape into a single polygon without making a decision about where to split it into multiple polygons.
If you want to make some sort of uniform polyhedron, these are best modeled deliberately.
For a more non-uniform/ organic looking crystal I recommend a more artistic approach. Radial symmetry can be used to create more deliberate jewel-cut patterns.
Try this:
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Start with a Dynamesh sphere of about medium resolution.
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Select the Clip Curve brush, and enable the Brush > Clip Brush Modifiers> Polygroup option. This will make every surface flattened by the clip brush into its own polygroup.
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Use the clip brush to flatten the shape facet by facet until you get the shape you want. Use ZRemesher with the “Keep Groups” function active to clean up the smashed geometry and create clean polygroup borders along the edges. Depending on how smashed the geometry is, you may first want to clean it up with Dynamesh before ZRemeshing.
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Once you have clean topology with each facet separated by a clean polygroup borders, you can use Geometry> Crease> CreasePG to instantly crease all polygroup edges. This will keep them crisp when being subdivided. If your geometry is completely planar and faceted with no curved surfaces, you can also simply disable the SMT button to keep it from smoothing during the Subdivision process.
If you have multiple “shards” cut this way, you can fuse them together with Live Boolean into more complex crsytaline structures.
