Abstract: | Anisotropic CdS nanorods tipped by Au nanoparticles on one edge (Au‐CdS‐NRs) are perpendicularly oriented at the air/water interface, whereby all the Au tips are located in the subphase, using the Langmuir–Blodgett technique. Since these nano‐objects reveal light‐induced charge separation at the semiconductor/metal interface, it is of high interest to control their organization. The orientation of these assemblies is studied in situ while compressing the Langmuir–Blodgett trough using the π‐A isotherm, Brewster angle microscopy, and horizontal touch voltammetry. All these analyses clearly confirm the induced organization of the amphiphilic Au‐CdS‐NRs by compression of the Langmuir layer. The compressed layers are successfully transferred by the Langmuir–Schaefer method onto transmission electron microscopy grids while maintaining the preferential orientation as analyzed by transmission, scanning and scanning trasmission electron microscopy, and X‐ray photoelectron spectroscopy. As far as can be determined, the Langmuir–Blodgett technique has not been used so far for perpendicularly orienting anisotropic nano‐objects. Moreover, these findings clearly demonstrate that anisotropic amphiphilic nano‐objects can be treated with some similarity to the traditional amphiphilic molecular building blocks. |