We present a detailed investigation of the resonator properties of high-quality rolled-up SiO2 optical microtubes reinforced by atomic layer deposition. The evolution of the resonant modes with increasing film thickness and the transition to a multimode regime, including higher order radial modes, is discussed. Measurements and simulations show that the higher order modes exhibit high optical quality and an increased extension of the evanescent field from the resonator into the surrounding matrix, making them a promising solution for future on-chip sensor applications with increased sensitivity.