bio-mimic interfaces with enantioselective properties remains challenging for chemists and materials scientists. For many research areas, such as medicine, biology, and chemistry, achieving enantioselective control is essential because it is a key parameter in molecular recognition. [5][6][7] Hence, the development of advanced methods to synthesize, separate, and detect chiral compounds is of particular importance.Chirality also plays a useful role in many nanosystems, [8] such as chiroptical molecular switches, [9][10][11] molecular motors, chiral surfaces, [12,13] chiral nanoparticles, [14][15][16][17][18][19] and chiral polymeric nanoparticles. [20][21][22] Overall, the areas of chiral nanoscience and nanotechnology hold exceptionally strong promise for further developments in areas such as catalysis, biorecognition, and chiral separation. Chiral mesoporous materials, for example, chiral mesoporous carbon, [23,24] chiral mesoporous silica, [25][26][27] and silica imprinted with different chiral functionalities, [28][29][30][31] are examples of promising nanosystems and have proved to play an important role in many fields of chemistry.One of the most promising chiral nanoscale systems is based on the use of chiral surfaces. Overall, there are three types of chiral surfaces, including surfaces from chiral bulk structures, such as quartz, and some high Miller-index surfaces of achiral crystals. [14] Chiral surfaces can also be produced by templating using chiral ligands and by the adsorption of chiral molecules to form chiral self-assembled monolayers (SAMs). [32][33][34][35] A potentially promising method to produce chiral surfaces is molecular layer deposition (MLD), used in combination with atomic layer deposition (ALD). [36] The A/MLD (atomic/molecular layer deposition) method is based on bifunctional compounds that vaporize, chemisorb, and react with a suitably functionalized surface. Both ALD and MLD allow the temporal separation of any number of precursors, each of which undergoes a self-limiting adsorption/ reaction on the surface so that the typical uptake is limited to approximately one monolayer of any given precursor. The ALD and MLD system is the same. However, the difference between these two is by replacing the small oxidizing precursor (e.g., water, O 3 ) used for ALD with oxidizing organic molecule as the reactant. Therefore, it will grow molecular layer instead of growing atomic layer. This leads to a growth controlled at the Atomic and molecular layer deposition (ALD and MLD) are techniques based on surface-directed self-limiting reactions that afford deposition of films controlled at the monolayer level and with extreme conformality, even on ultra-high-aspect-ratio and porous substrates. These methodologies are typically used to deposit thin films with desirable physical properties and functionality. Here, the MLD process is harnessed to demonstrate the growth of molecularly thin chiral films that inherit a desirable chemical property directly from the source precursor: using this innovative t...