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Increased usage of gold nanorods (AuNRs) in various biosensing and medical applications requires tight size and morphology control. This is often achieved by tuning the aggregation behavior of the stabilizing ligand cetrimonium bromide (CTAB). Because the role of CTAB during AuNR growth is still a matter of debate, simultaneous small‐angle X‐ray and neutron scattering experiments (SAXS/SANS) and measurements are performed. The SAXS/SANS measurements have enabled an instantaneous correlation between the size of evolving AuNR and the nanostructure of guiding CTAB moieties. Upon modifying the aggregation behavior of CTAB micelles by adding hexanol or pentanol as inert additives in the precursor solution, a marked change in reaction kinetics is observed. Alcohol‐modified CTAB nanostructures have improved AuNR size uniformity compared to those prepared in alcohol‐free CTAB solutions, which are attributed to different growth modes. The change in reaction kinetics is linked to a changed stabilization mechanism of reactants and nascent AuNR facilitated by CTAB micelles. [ABSTRACT FROM AUTHOR]