Metal–organic frameworks (MOFs) are a rather new class of crystalline, nanoporous solids that are self‐assembled from inorganic, metal or metal‐oxo nodes and organic linkers. Powder MOFs are originally developed for gas storage and catalyst applications, but more recently, more advanced applications have used well‐defined MOF thin films in electronic, photonic, and sensing devices. MOF thin films for targeted applications can be fabricated on appropriately functionalized substrates using a programmed layer‐by‐layer (LbL) assembly technique, which yields oriented, highly crystalline MOF thin films (surface‐mounted MOFs, SURMOFs). The LbL assembly technique as well as the huge potential of SURMOFs is presented herein. Emerging SURMOF properties related to their heteroepitaxy, postsynthetic modification/crosslinking, lithography, and photoswitching are highlighted.