ORGANISMS such as diatoms and radiolaria synthesize elaborate biomineral exoskeletons which display hierarchical structures patterned on length scales from less than a micrometre to millimetres. Synthetic materials chemistry, in contrast, has traditionally been able to achieve regular patterning only on microscopic (<10 Angstrom) and more recently(1-3) mesoscopic (10-10(3) Angstrom) length scales. Here we report the synthesis of crystalline, lamellar aluminophosphate structures that are patterned on the submicrometre-to-millimetre scales found in the living world. As in the syntheses of ordered mesoporous solids(1-3), our approach involves templating by self-assembled organic aggregates, and we propose that the larger scale of the patterning here arises from the involvement of vesicle templates rather than the micelle-like or bilayer structures thought to be responsible for mesoscale pattern formation(1-3).