Optical properties of MOF supraparticles. a)–d) Top row: FESEM of RD‐ZIF‐8 (a), TRD‐ZIF‐8 (b), C‐ZIF‐8 (c) and O‐UiO‐66 (d) supraparticles, exhibiting structural coloration from the interaction of the incident light and the supraparticle structure (optical microscopy images in inset). Middle row: magnification of the particle surfaces, showing well‐ordered arrangements of the primary particles; bottom row: reflection spectra measured for individual supraparticles. e) Effect of supraparticle size on the intensity of the photonic stop band, exemplarily shown for TRD‐ZIF‐8 supraparticles. f) Relationship between size and shape of the primary particles on the wavelength of the reflection peak, measured in suspension. g) Angle‐dependent reflectance spectra of MOF supraparticles consisting of the same colloidal particle size but different shapes, along with corresponding photographs showing the observable coloration. h) FESEM of spherical and buckled MOF supraparticles, with optical microscopy images showing differences in structural color. The surface of the buckled supraparticle shows the hexagonally‐packed particle layer. i) Reflectance spectra of individual spherical and buckled MOF supraparticles. j) Reflectance spectra of spherical and buckled supraparticles measured in suspension.