This research provides a flexible approach to manipulate formation of InGaAs nanostructures on the GaAs (100) surface by varying arsenic (As4) beam equivalent pressure (BEP). By selecting the As4/(In+Ga) BEP ratio to be 4, 8, 20, 50 and 100, we were able to obtain different quantum structures from quantum well (QW) to quantum dots (QDs), then to spatially ordered quantum dot chains (QD-chains), and finally to quantum wires (QWRs), respectively. This transformation of nanostructures was explained by anisotropic surface diffusion coupled with the strain relieving Stranski–Krastanov growth mode, while the anisotropy was modulated by increasing As4 flux and subsequently enhanced by multilayer-stacking growth with a suitable spacer thickness. Photoluminescence characteristics show correlation to the nanostructure morphology for each sample. In particular, the formation of QD-chains and QWRs results in anisotropic features that offer potential device applications.