We describe the growth and characterization of 10 nm to 10 micron-scale islands created by depositing Ag onto Si(111) at elevated temperatures. By varying the surface coverage of Ag, we are able to produce and control the distribution of Ag(111) and/or Ag(100) single-crystal islands. These were examined using scanning tunneling microscopy (STM), X-ray diffraction (XRD), helium ion microscopy (HIM), and atomic force microscopy. The formation of 3D islands with orientations of either ( 111) or (100) was confirmed by STM and XRD analysis. As these islands manifest as tiny single crystals of elemental Ag, they can be ideally used as low-cost or disposable substrates to host molecular architectures; we demonstrate this by comparing absorption and thermal behavior of 1,3,5-benzenetricarboxylic acid molecules on the islands and noting identical behavior and reactivity to experiments performed on Ag single-crystal counterparts. These islands provide an economical and practical method for facilitating molecular adsorption on two distinct microsubstrates at the same time while under identical experimental conditions.