DOI: 10.1002/adma. 201401940 sensing,[13] batteries,[14] supercapacitors [15] and electrochromic devices—a more desirable form may be thin films.[16–18] Several approaches to MOF thin-film formation have now been explored, at least in preliminary fashion. The approaches include: surface-initiated solvothermal growth,[19–21] layer-bylayer assembly (also termed liquid-phase epitaxy),[22–24] substrate corrosion and/or reactive electrodeposition,[25–28] microwave-induced thermal deposition [29] and dip coating from colloidal solutions.[30] While each has its virtues, none has yet proven universally applicable or nearly so. Thus, there is a need for additional deposition methods—especially ones that are simple and broadly applicable, or at least applicable to MOFs that appear poorly suited to the methods noted above. Electrophoretic deposition (EPD) is a well-established technique for fabricating thin films, especially from nanoparticulate building blocks. The application of a DC electric field to a suspension of charged particles in a nonpolar solvent can result in particle transport and deposition onto a conductive substrate. EPD has previously been employed to deposit semiconducting,[31–35] metallic [36–38] and insulating [39, 40] nanoparticles on conductive platforms. Here we report the electrophoresis-driven formation and growth of MOF thin films. The potential generality of the EPD method was demonstrated by the successful deposition of four representative MOFs: the Zr-based materials, NU-1000 [41] and UiO-66 [42](see Figure 1a and b); the iconic Cu-based MOF, HKUST-1;[43] and the aluminum-based form of MIL-53 [44](see Figures S1 and S2). Notably, the deposited materials are characterized by distinctly different topologies, porosities, morphologies, sizes of crystallites, and degrees of chemical stability. During the material synthesis, all 4 types of MOFs present some surface defects (possibly due to missing linkers or missing metal nodes) that will give rise to some partial charges on the surface of the MOFs. During EPD process, those partial charges drive the particles toward the oppositely charged electrode. In practice, all of the examined MOFs display net negative charges and were deposited on the positively charged electrode. When the polarity of the electrodes was switched, as expected, the MOF particles were deposited on the opposite electrode, supporting the fact that the charged surfaces of the MOF materials drive their deposition. Finally, to further test the usefulness of EPD, we examined the feasibility of: a) depositing micropatterned films, and b) depositing two types of MOFs on a single conductive support.