QRs), [4,5] have been considered as promising light-emitting components in modern display, lighting, bioimaging, and photonics applications. [6][7][8][9][10][11][12][13][14][15][16] Based on the quantum-confinement effect, these nanocrystals possess outstanding optical properties, such as precisely tunable emission, narrow emission bandwidths, high photoluminescence (PL) quantum yields (QYs), and better photostability compared to molecular dyes. [17][18][19] In addition, 1D anisotropic nanocrystals, such as CdSe/CdS core/shell QRs with a dot-in-rod geometry, show strongly polarized absorption and emission along the long axis of the QR. [20][21][22] The ability of strongly emitting semiconductor QR, when macroscopically aligned, to emit linearly polarized light makes them perfect candidate for liquid crystal display (LCD) backlights. To translate their anisotropic properties from a single nanocrystal to the macroscopically polarized lightemitting materials, QRs need to be oriented unidirectionally in plane, which can be achieved by several assembly approaches. [23][24][25][26][27] Our previous work has introduced photoinduced alignment of QRs in a liquid crystal polymer (LCP) matrix as a strategy to control QR orientation from centimeter [28] down to micrometer domain sizes. [29] By utilizing the photoactive sulfonic azo dye as an alignment layer, photo alignment is transferred to the liquid crystal monomers (LCM), whose reorientation results in torque that is transferred to the QRs through the repulsive interactions with the QR capping ligands. In general, the longchain organic ligands are used to protect/functionalize the surface and increase the steric repulsion of semiconductor QRs. It was observed that in the QR/LCM composite systems, the interaction of the QR ligands with the molecular LC matrix often leads to topological defects in the QRs/LCP composite films, which also depends on the concentrations of both nanoparticles and LCM in solution. [30][31][32][33][34] On one hand, for the low concentration of LC molecules, the orientational forces do not notably contribute to the aggregation process, but the interaction due to the change of the order parameter near the QR surface plays an important role. [35,36] This process also induces deformation of the LC director along the surface of the colloid The ability of strongly emitting semiconductor quantum rods (QRs), when macroscopically aligned, to emit linearly polarized light makes them the perfect candidate for liquid crystal (LC) display backlights. Macroscopic QR ordering is previously demonstrated by photoalignment of QR composites with polymerizable LC monomers. In this study, it is demonstrated that the optimum concentration of LC monomers and core/shell CdSe/CdS QRs enabling someone to achieve their uniform homogeneous orientation in photoaligned films strongly depends on the lengths and aspect ratios of the QRs. By aligning QRs with different aspect ratios ranging from 3 to 10, the best performance is achieved for shorter QRs with lengths of 11 and 31 ...