The ability of alkylthiol capped gold nanoparticles (Au NPs) to tune, alter, and reverse the alignment of nematic liquid crystals (LCs) has been investigated in detail. Adjusting the concentration of the suspended Au NPs in the nematic LC host, optimizing the sample preparation protocol, or providing different sample substrates (untreated glass slides, rubbed polyimide-coated LC test cell, or ITO-coated glass slides) results in several LC alignment scenarios (modes) including vertical alignment, planar alignment, and a thermally controlled alignment switch between these two alignment modes. The latter thermal switch between planar and homeotropic alignment was observed particularly for lower concentrations (i.e., around 1 to 2 wt %) of suspended NPs in the size regime of 1.5-2 nm and was found to be concentration-dependent and thermally reversible. Different scenarios are discussed that could explain these induced alignment modes. In one scenario, the NP-induced alignment is related to the temperature-dependent change of the order parameter, S, of the nematic phase (ordering in the bulk). In the second scenario, a change of the ordering of the nematic molecules around the NPs that reside at the interfaces is described. We also started to test spin coating as an alternative way of preparing nematic thin films with well-separated Au NPs on the substrate and found this to be a possible method for manufacturing of future NP-doped LC devices, as this method produced evenly distributed NPs on glass substrates. Together the presented findings continue to pave the way for LC display-related applications of Au NP-doped nematic LCs and provide insights for N-LC sensor applications.