Fully oriented and functional MOF-on-MOF films were achieved by epitaxial growth in solution. In their Communication on page 6886 ff., M. Takahashi, C. J. Doonan, and co-workers exploited the alignment of MOF multilayer films on an oriented Cu(OH)2 film. Ag nanoparticles accommodated in aligned pores with anisotropic shape in the selective layer of MOF-on-MOF film showed unique anisotropic plasmon resonances.