Concept:
Crystalline glazes are specialty glazes where large, visible macro-crystals grow within the glassy matrix during a very specific, controlled cooling cycle in the kiln.
Step 1:
For crystals to grow in a glaze, the glaze melt must be highly fluid (low in alumina) and supersaturated with a specific mineral that will crystallize out as the temperature drops.
Step 2:
The classic and most reliable macro-crystalline glazes are based on Willemite crystals. Willemite is a zinc silicate mineral.
Step 3:
To create Willemite crystals, the glaze recipe must contain massive amounts of Zinc Oxide ($ZnO$)—often up to 25% or 30% of the recipe—combined with Silica. During the cooling cycle, the zinc and silica bond to form the large, beautiful starburst or floral-shaped crystals.
Step 4:
While Titanium Oxide can act as a "seed" to help crystals start growing, Zinc Oxide is the actual primary building block (the most favorable and necessary oxide) for the large crystals themselves.
Step 5:
Because Zinc is the fundamental element required to form Willemite crystals, Zinc Oxide is the correct answer.
\[
\boxed{\text{(4) Zinc Oxide}}
\]