Symmetric droplet-etched quantum dots (QDs) are the leading candidate for generating high-performance polarization-entangled photon pairs. One of the challenges is how to precisely engineer the properties of QDs by controlling the morphology of etched nanoholes. In this paper, we systematically investigate the influence of the underlying material, showing the morphological evolution of the nanohole structure as well as symmetric GaAs QDs with an average fine-structure splitting (FSS) of (5.9 ± 1.2) μeV. Moreover, we develop a theoretical model that quantitatively reproduces the experimental data and provides insights into the mechanisms governing the relationship between the anisotropy of nanoholes in the [Formula: see text] crystallographic direction and the growth parameters. Our theoretical analysis also indicates how to improve the symmetry of nanoholes to meet the requirements for implementing QDs in entangled photon sources.