Crystal tectonics involves the chemical-based construction and self-assembl
y of organized materials from solid-state building blocks, such as inorgani
c nanoparticles. This Perspective describes, through a series of examples,
how the architectural complexity of materials with higher-order structure c
an be controlled by organic templating, interparticle molecular recognition
and mesophase transformation. It is shown how the coupling of synthesis an
d self-assembly over multiple length scales is leading to new horizons in t
he chemistry of organized matter.