Ultra-low loss optical thin films find broad applications in fields such as vertical-cavity surface-emitting lasers and optical atomic clocks. The main optical losses in AlGaAs/GaAs distributed Bragg reflectors (DBRs) prepared using metal-organic chemical vapor deposition (MOCVD) arise from absorption loss caused by free carriers within the layers and scattering loss caused by surface roughness. In this study, we fabricated AlGaAs and GaAs single-layer thin films with varying Al compositions on substrates of three crystal orientations and under different V/III ratios. The dependence of carrier concentration and surface morphology on different substrates and growth conditions was investigated. Thin films grown on substrates with three different crystal orientations exhibited three distinct growth modes (step-flow mode, SK mode, and FM mode). The impact of the V/III ratio on the growth mode was found to be complex. Higher V/III ratios resulted in poorer morphology for films grown on (100) substrates, while better morphology was observed on (211) B substrates. Furthermore, the surface morphology of films grown on (100) 15° off substrates showed less sensitivity to changes in the V/III ratio. With increasing Al composition, the carrier concentration of the films significantly increased. Elevating the V/III ratio proved effective in suppressing the incorporation of carbon, thereby reducing the carrier concentration of AlGaAs films. GaAs films exhibited a low carrier concentration at an appropriate V/III ratio. Additionally, the distinct abilities of different substrates to adsorb impurities exerted a significant impact on the carrier concentration of the films. This study demonstrates that, under optimal conditions, it is feasible to fabricate AlGaAs/GaAs Bragg mirrors with low carrier concentration and relatively small roughness on (100) 15° off substrates.