Layered
nanomaterials fascinate researchers for their mechanical,
barrier, optical, and transport properties. Nacre is a biological
example thereof, combining excellent mechanical properties by aligned
submicron inorganic platelets and nanoscale proteinic interlayers.
Mimicking nacre with advanced nanosheets requires ultraconfined organic
layers aimed at nacre-like high reinforcement fractions. We describe
inorganic/polymer hybrid Bragg stacks with one or two fluorohectorite
clay layers alternating with one or two poly(ethylene glycol) layers.
As indicated by X-ray diffraction, perfect one-dimensional crystallinity
allows for homogeneous single-phase materials with up to a 84% clay
volume fraction. Brillouin light spectroscopy allows the exploration
of ultimate mechanical moduli without disturbance by flaws, suggesting
an unprecedentedly high Young’s modulus of 162 GPa along
the aligned clays, indicating almost ideal reinforcement under these
conditions. Importantly, low heat conductivity is observed across
films, κ
⊥
= 0.11–0.15 W m
–1
K
–1
, with a high anisotropy of κ
∥
/κ
⊥
= 28–33. The macroscopic mechanical
properties show ductile-to-brittle change with an increase in the
clay volume fraction from 54% to 70%. Conceptually, this work reveals
the ultimate elastic and thermal properties of aligned layered clay
nanocomposites in flaw-tolerant conditions.