The design of multifunctional molecular devices is an expanding frontier area of research encompassing the fields of materials science, nanotechnology, and supramolecular chemistry [1][2][3]. A current theme is to design molecules with individual components that operate independently of one another, yet work cooperatively as a team to produce devices with greater function than the sum of their individual parts [4][5][6]. Molecules with the capacity to perform a variety of stimuli-responsive functions based on built-in algorithms can, therefore, independently process information, and then of their own accord, provide a composite result autonomously [7][8][9][10][11][12][13][14][15][16][17]. Molecules with the ability to perform Boolean algebraic operations are the focus of this chapter.Intelligent molecular systems designed to be activated by some external stimulus by changing a physical or chemical state can be viewed as switches, and therefore, may be useful for the transfer, processing, and storage of information. Dozens of research laboratories around the world have embraced the design, synthesis, characterization, and testing of chemical systems that mimic the basic operations of electrical circuitry [18]. The general engineering approach to designing information-processing molecules is based on a modular strategy with specific units of structural and functional importance [19]. Earlier reviews described in detail the various strategies for designing luminescence sensing devices: these ideas range in scope from ways of covalently arranging modular units to the exploitation of self-assembly [20][21][22].This multidisciplinary research field demands a number of skill sets from a background in organic synthesis for the strategic design and molecular engineering of novel chemical systems, to analytical chemistry for the quantification of analyte concentrations and the determination of binding constants, as well as other thermodynamic and kinetic parameters, and Boolean algebra and binary computation for expressing observed chemical phenomena (analog information) as easy-to-interpret digital information. Then, there are also the skills and tools required for anchoring these molecular devices at interfaces and surfaces.