Hybrid films were fabricated via a LbL-SC approach from GO and rod-or plate-shaped TNCs. GO was prepared using a modified Hummers method. The TNCs were synthesized following the protocol by Gordon et al. Figure ) shows an SEM image of the freeze-dried GO sheets (∼1.1 nm thickness, up to ∼5 µm sheet size, cf. Supporting Information, Section S2). Figures and) present TEM images of brookite/anatase TNRs (∼40 nm length) and anatase TNPs (∼22 nm edge length), respectively. Data of the XRD characterization of the nanocrystals can be found in the Supporting Information, Section S1. The hybrid film fabrication process is schematically illustrated in Figure ). First, 2×25 µL of a methanolic/aqueous GO solution (∼0.1 wt%) was applied onto a rotating substrate, e.g., quartz slides, PI foil, or silicon wafers, followed by the deposition of the TNCs from their colloidal solution in chloroform (0.05-0.4 wt%, 1×25 µL), and the subsequent deposition of 2×25 µL GO solution, yielding a sandwiched hybrid film. By varying the number of alternating deposition cycles, the film thickness and composition was adjusted. The SEM image (Figure ), inset) shows the cross-section of a multilayered GO/TNR hybrid film formed by applying 10 SC deposition cycles. Figures ) show SEM images of GO/TNP and GO/TNR films deposited on silicon wafers, respectively. At the edges of the film, the incorporation of TNCs between GO layers is clearly seen. The LbL-SC deposition of the films was monitored via UV-vis absorption spectroscopy. Figures ) show the absorbance spectra of GO/TNP and GO/TNR films deposited on quartz substrates. The spectra were recorded at four different positions of each film and averaged. The shaded areas correspond to the standard deviation of four measurements, indicating a homogeneous film deposition on the substrates.